Articles | Volume 20, issue 12
https://doi.org/10.5194/acp-20-7335-2020
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-20-7335-2020
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
25 Jun 2020
Research article |
| 25 Jun 2020
| 25 Jun 2020
Evaluating the impact of blowing-snow sea salt aerosol on springtime BrO and O3 in the Arctic
Jiayue Huang
Department of Atmospheric Sciences, University of Washington, Seattle, WA 98115, USA
Lyatt Jaeglé
CORRESPONDING AUTHOR
Department of Atmospheric Sciences, University of Washington, Seattle, WA 98115, USA
Qianjie Chen
Department of Atmospheric Sciences, University of Washington, Seattle, WA 98115, USA
now at: Department of Chemistry, University of Michigan, Ann Arbor,
MI 48109, USA
Becky Alexander
Department of Atmospheric Sciences, University of Washington, Seattle, WA 98115, USA
Tomás Sherwen
Wolfson Atmospheric Chemistry Laboratories, Department of Chemistry, University of York, York YO10 5DD, UK
National Centre for Atmospheric Science, University of York, York,
YO10 5DD, UK
Mat J. Evans
Wolfson Atmospheric Chemistry Laboratories, Department of Chemistry, University of York, York YO10 5DD, UK
National Centre for Atmospheric Science, University of York, York,
YO10 5DD, UK
Nicolas Theys
Royal Belgian Institute for Space Aeronomy (BIRA-IASB), Brussels,
Belgium
Sungyeon Choi
Science Systems and Applications, Inc., Lanham, MD 20706, USA
NASA Goddard Space Flight Center, Greenbelt, MD 20771, USA
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Yutao Chen, Ronald J. van der A, Jieying Ding, Henk Eskes, Jason E. Williams, Nicolas Theys, Athanasios Tsikerdekis, and Pieternel F. Levelt
EGUsphere, https://doi.org/10.5194/egusphere-2024-1094, https://doi.org/10.5194/egusphere-2024-1094, 2024
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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There is a lack of local SO2 top-down emission inventories in India. With the improvement in the divergence method and the derivation of SO2 local lifetime, gridded SO2 emissions over a large area can be estimated efficiently. This method can be applied to any region in the world to derive SO2 emissions. Especially for regions with high latitudes, our methodology has the potential to significantly improve the top-down derivation of SO2 emission estimates.
Fei Liu, Steffen Beirle, Joanna Joiner, Sungyeon Choi, Zhining Tao, K. Emma Knowland, Steven J. Smith, Daniel Q. Tong, Siqi Ma, Zachary T. Fasnacht, and Thomas Wagner
Atmos. Chem. Phys., 24, 3717–3728, https://doi.org/10.5194/acp-24-3717-2024, https://doi.org/10.5194/acp-24-3717-2024, 2024
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Using satellite data, we developed a coupled method independent of the chemical transport model to map NOx emissions across US cities. After validating our technique with synthetic data, we charted NOx emissions from 2018–2021 in 39 cities. Our results closely matched EPA estimates but also highlighted some inconsistencies in both magnitude and spatial distribution. This research can help refine strategies for monitoring and managing air quality.
Linia Tashmim, William C. Porter, Qianjie Chen, Becky Alexander, Charles H. Fite, Christopher D. Holmes, Jeffrey R. Pierce, Betty Croft, and Sakiko Ishino
Atmos. Chem. Phys., 24, 3379–3403, https://doi.org/10.5194/acp-24-3379-2024, https://doi.org/10.5194/acp-24-3379-2024, 2024
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Dimethyl sulfide (DMS) is mostly emitted from ocean surfaces and represents the largest natural source of sulfur for the atmosphere. Once in the atmosphere, DMS forms stable oxidation products such as SO2 and H2SO4, which can subsequently contribute to airborne particle formation and growth. In this study, we update the DMS oxidation mechanism in the chemical transport model GEOS-Chem and describe resulting changes in particle growth as well as the overall global sulfur budget.
Kelvin H. Bates, Mathew J. Evans, Barron H. Henderson, and Daniel J. Jacob
Geosci. Model Dev., 17, 1511–1524, https://doi.org/10.5194/gmd-17-1511-2024, https://doi.org/10.5194/gmd-17-1511-2024, 2024
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Accurate representation of rates and products of chemical reactions in atmospheric models is crucial for simulating concentrations of pollutants and climate forcers. We update the widely used GEOS-Chem atmospheric chemistry model with reaction parameters from recent compilations of experimental data and demonstrate the implications for key atmospheric chemical species. The updates decrease tropospheric CO mixing ratios and increase stratospheric nitrogen oxide mixing ratios, among other changes.
Bruno Franco, Lieven Clarisse, Nicolas Theys, Juliette Hadji-Lazaro, Cathy Clerbaux, and Pierre Coheur
EGUsphere, https://doi.org/10.5194/egusphere-2023-2707, https://doi.org/10.5194/egusphere-2023-2707, 2023
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Using IASI global infrared measurements, we retrieve nitrous acid (HONO) in fire plumes from space. We detect large enhancements of pyrogenic HONO worldwide, especially from intense wildfires at North Hemisphere mid and high latitudes. Predominance of IASI's nighttime over daytime measurements sheds light on HONO's extended lifetime and secondary formation during long-range transport in smoke plumes. Our findings deepen the understanding of atmospheric HONO, crucial for air quality assessment.
Vitali E. Fioletov, Chris A. McLinden, Debora Griffin, Nickolay A. Krotkov, Can Li, Joanna Joiner, Nicolas Theys, and Simon Carn
Atmos. Meas. Tech., 16, 5575–5592, https://doi.org/10.5194/amt-16-5575-2023, https://doi.org/10.5194/amt-16-5575-2023, 2023
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Snow-covered terrain, with its high reflectance in the UV, typically enhances satellite sensitivity to boundary layer pollution. However, a significant fraction of high-quality cloud-free measurements over snow is currently excluded from analyses. In this study, we investigated how satellite SO2 measurements over snow-covered surfaces can be used to improve estimations of annual SO2 emissions.
Ryan J. Pound, Lucy V. Brown, Mat J. Evans, and Lucy J. Carpenter
EGUsphere, https://doi.org/10.5194/egusphere-2023-2447, https://doi.org/10.5194/egusphere-2023-2447, 2023
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Iodine-mediated loss of ozone to the ocean surface and the subsequent emission of iodine species has a large effect on the troposphere. Here we combine recent experimental insights to develop a box model of the process, which we then parameterise and incorporate into the GEOS-Chem transport model. We find that these new insights have a small impact on the total emission of iodine but significantly change its distribution.
Adedayo R. Adedeji, Stephen J. Andrews, Matthew J. Rowlinson, Mathew J. Evans, Alastair C. Lewis, Shigeru Hashimoto, Hitoshi Mukai, Hiroshi Tanimoto, Yasunori Tohjima, and Takuya Saito
Atmos. Chem. Phys., 23, 9229–9244, https://doi.org/10.5194/acp-23-9229-2023, https://doi.org/10.5194/acp-23-9229-2023, 2023
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We use the GEOS-Chem model to interpret observations of CO, C2H6, C3H8, NOx, NOy and O3 made from Hateruma Island in 2018. The model captures many synoptic-scale events and the seasonality of most pollutants at the site but underestimates C2H6 and C3H8 during the winter. These underestimates are unlikely to be reconciled by increases in biomass burning emissions but could be reconciled by increasing the Asian anthropogenic source of C2H6 and C3H8 by factors of around 2 and 3, respectively.
Zhouxing Zou, Qianjie Chen, Men Xia, Qi Yuan, Yi Chen, Yanan Wang, Enyu Xiong, Zhe Wang, and Tao Wang
Atmos. Chem. Phys., 23, 7057–7074, https://doi.org/10.5194/acp-23-7057-2023, https://doi.org/10.5194/acp-23-7057-2023, 2023
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We present OH observation and model simulation results at a coastal site in Hong Kong. The model predicted the OH concentration under high-NOx well but overpredicted it under low-NOx conditions. This implies an insufficient understanding of OH chemistry under low-NOx conditions. We show evidence of missing OH sinks as a possible cause of the overprediction.
Jean-Paul Vernier, Thomas Aubry, Claudia Timmreck, Anja Schmidt, Lieven Clarisse, Fred Prata, Nicolas Theys, Andrew Prata, Graham Mann, Hyundeok Choi, Simon Carn, Richard Rigby, Susan Loughlin, and John Stevenson
EGUsphere, https://doi.org/10.5194/egusphere-2023-1116, https://doi.org/10.5194/egusphere-2023-1116, 2023
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The 2019 Raikoke eruption (Kamchatka, Russia) generated one of the largest emissions of particles and gases into stratosphere since the 1991 Mt Pinatubo eruption. The Volcano Response initiative, an international effort provided a platform for the community to share information about this eruption. We show that this effect led to a minor global surface cooling of 0.02 Celsius in 2020, which is negligible relative to warming induced by human greenhouse gas emissions.
Zhuang Jiang, Becky Alexander, Joel Savarino, and Lei Geng
EGUsphere, https://doi.org/10.5194/egusphere-2023-1054, https://doi.org/10.5194/egusphere-2023-1054, 2023
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Ice-core nitrate could track the past atmospheric NOx and oxidant level, but its interpretation is hampered by the post-depositional processing. In this work, an inverse model was developed and tested against two polar sites, and was shown to well reproduce the observed nitrate signals in snow and atmosphere, suggesting that the model can properly correct for the effect of post-depositional processing. This model offers a very useful tool for future studies on ice-core nitrate records.
Thomas Wagner, Simon Warnach, Steffen Beirle, Nicole Bobrowski, Adrian Jost, Janis Puķīte, and Nicolas Theys
Atmos. Meas. Tech., 16, 1609–1662, https://doi.org/10.5194/amt-16-1609-2023, https://doi.org/10.5194/amt-16-1609-2023, 2023
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We investigate 3D effects of volcanic plumes on the retrieval results of satellite and ground-based UV–Vis observations. With its small ground pixels of 3.5 x 5.5 km², the TROPOMI instrument can detect much smaller volcanic plumes than previous instruments. At the same time, 3D effects become important. The effect of horizontal photon paths especially can lead to a strong underestimation of the derived plume contents of up to > 50 %, which can be further increased for strong absorbers like SO2.
Viral Shah, Daniel J. Jacob, Ruijun Dang, Lok N. Lamsal, Sarah A. Strode, Stephen D. Steenrod, K. Folkert Boersma, Sebastian D. Eastham, Thibaud M. Fritz, Chelsea Thompson, Jeff Peischl, Ilann Bourgeois, Ilana B. Pollack, Benjamin A. Nault, Ronald C. Cohen, Pedro Campuzano-Jost, Jose L. Jimenez, Simone T. Andersen, Lucy J. Carpenter, Tomás Sherwen, and Mat J. Evans
Atmos. Chem. Phys., 23, 1227–1257, https://doi.org/10.5194/acp-23-1227-2023, https://doi.org/10.5194/acp-23-1227-2023, 2023
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NOx in the free troposphere (above 2 km) affects global tropospheric chemistry and the retrieval and interpretation of satellite NO2 measurements. We evaluate free tropospheric NOx in global atmospheric chemistry models and find that recycling NOx from its reservoirs over the oceans is faster than that simulated in the models, resulting in increases in simulated tropospheric ozone and OH. Over the U.S., free tropospheric NO2 contributes the majority of the tropospheric NO2 column in summer.
Vitali E. Fioletov, Chris A. McLinden, Debora Griffin, Ihab Abboud, Nickolay Krotkov, Peter J. T. Leonard, Can Li, Joanna Joiner, Nicolas Theys, and Simon Carn
Earth Syst. Sci. Data, 15, 75–93, https://doi.org/10.5194/essd-15-75-2023, https://doi.org/10.5194/essd-15-75-2023, 2023
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Sulfur dioxide (SO2) measurements from three satellite instruments were used to update and extend the previously developed global catalogue of large SO2 emission sources. This version 2 of the global catalogue covers the period of 2005–2021 and includes a total of 759 continuously emitting point sources. The catalogue data show an approximate 50 % decline in global SO2 emissions between 2005 and 2021, although emissions were relatively stable during the last 3 years.
Simone T. Andersen, Beth S. Nelson, Katie A. Read, Shalini Punjabi, Luis Neves, Matthew J. Rowlinson, James Hopkins, Tomás Sherwen, Lisa K. Whalley, James D. Lee, and Lucy J. Carpenter
Atmos. Chem. Phys., 22, 15747–15765, https://doi.org/10.5194/acp-22-15747-2022, https://doi.org/10.5194/acp-22-15747-2022, 2022
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The cycling of NO and NO2 is important to understand to be able to predict O3 concentrations in the atmosphere. We have used long-term measurements from the Cape Verde Atmospheric Observatory together with model outputs to investigate the cycling of nitrogen oxide (NO) and nitrogen dioxide (NO2) in very clean marine air. This study shows that we understand the processes occurring in very clean air, but with small amounts of pollution in the air, known chemistry cannot explain what is observed.
Qianjie Chen, Jessica A. Mirrielees, Sham Thanekar, Nicole A. Loeb, Rachel M. Kirpes, Lucia M. Upchurch, Anna J. Barget, Nurun Nahar Lata, Angela R. W. Raso, Stephen M. McNamara, Swarup China, Patricia K. Quinn, Andrew P. Ault, Aaron Kennedy, Paul B. Shepson, Jose D. Fuentes, and Kerri A. Pratt
Atmos. Chem. Phys., 22, 15263–15285, https://doi.org/10.5194/acp-22-15263-2022, https://doi.org/10.5194/acp-22-15263-2022, 2022
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During a spring field campaign in the coastal Arctic, ultrafine particles were enhanced during high wind speeds, and coarse-mode particles were reduced during blowing snow. Calculated periods blowing snow were overpredicted compared to observations. Sea spray aerosols produced by sea ice leads affected the composition of aerosols and snowpack. An improved understanding of aerosol emissions from leads and blowing snow is critical for predicting the future climate of the rapidly warming Arctic.
William F. Swanson, Chris D. Holmes, William R. Simpson, Kaitlyn Confer, Louis Marelle, Jennie L. Thomas, Lyatt Jaeglé, Becky Alexander, Shuting Zhai, Qianjie Chen, Xuan Wang, and Tomás Sherwen
Atmos. Chem. Phys., 22, 14467–14488, https://doi.org/10.5194/acp-22-14467-2022, https://doi.org/10.5194/acp-22-14467-2022, 2022
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Radical bromine molecules are seen at higher concentrations during the Arctic spring. We use the global model GEOS-Chem to test whether snowpack and wind-blown snow sources can explain high bromine concentrations. We run this model for the entire year of 2015 and compare results to observations of bromine from floating platforms on the Arctic Ocean and at Utqiaġvik. We find that the model performs best when both sources are enabled but may overestimate bromine production in summer and fall.
Miriam Latsch, Andreas Richter, Henk Eskes, Maarten Sneep, Ping Wang, Pepijn Veefkind, Ronny Lutz, Diego Loyola, Athina Argyrouli, Pieter Valks, Thomas Wagner, Holger Sihler, Michel van Roozendael, Nicolas Theys, Huan Yu, Richard Siddans, and John P. Burrows
Atmos. Meas. Tech., 15, 6257–6283, https://doi.org/10.5194/amt-15-6257-2022, https://doi.org/10.5194/amt-15-6257-2022, 2022
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The article investigates different S5P TROPOMI cloud retrieval algorithms for tropospheric trace gas retrievals. The cloud products show differences primarily over snow and ice and for scenes under sun glint. Some issues regarding across-track dependence are found for the cloud fractions as well as for the cloud heights.
Yanzhi Cao, Zhuang Jiang, Becky Alexander, Jihong Cole-Dai, Joel Savarino, Joseph Erbland, and Lei Geng
Atmos. Chem. Phys., 22, 13407–13422, https://doi.org/10.5194/acp-22-13407-2022, https://doi.org/10.5194/acp-22-13407-2022, 2022
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We investigate the potential of ice-core preserved nitrate isotopes as proxies of stratospheric ozone variability by measuring nitrate isotopes in a shallow ice core from the South Pole. The large variability in the snow accumulation rate and its slight increase after the 1970s masked any signals caused by the ozone hole. Moreover, the nitrate oxygen isotope decrease may reflect changes in the atmospheric oxidation environment in the Southern Ocean.
Nicolas Theys, Christophe Lerot, Hugues Brenot, Jeroen van Gent, Isabelle De Smedt, Lieven Clarisse, Mike Burton, Matthew Varnam, Catherine Hayer, Benjamin Esse, and Michel Van Roozendael
Atmos. Meas. Tech., 15, 4801–4817, https://doi.org/10.5194/amt-15-4801-2022, https://doi.org/10.5194/amt-15-4801-2022, 2022
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Sulfur dioxide plume height after a volcanic eruption is an important piece of information for many different scientific studies and applications. Satellite UV retrievals are useful in this respect, but available algorithms have shown so far limited sensitivity to SO2 height. Here we present a new technique to improve the retrieval of SO2 plume height for SO2 columns as low as 5 DU. We demonstrate the algorithm using TROPOMI measurements and compare with other height estimates.
Pieternel F. Levelt, Deborah C. Stein Zweers, Ilse Aben, Maite Bauwens, Tobias Borsdorff, Isabelle De Smedt, Henk J. Eskes, Christophe Lerot, Diego G. Loyola, Fabian Romahn, Trissevgeni Stavrakou, Nicolas Theys, Michel Van Roozendael, J. Pepijn Veefkind, and Tijl Verhoelst
Atmos. Chem. Phys., 22, 10319–10351, https://doi.org/10.5194/acp-22-10319-2022, https://doi.org/10.5194/acp-22-10319-2022, 2022
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Using the COVID-19 lockdown periods as an example, we show how Sentinel-5P/TROPOMI trace gas data (NO2, SO2, CO, HCHO and CHOCHO) can be used to understand impacts on air quality for regions and cities around the globe. We also provide information for both experienced and inexperienced users about how we created the data using state-of-the-art algorithms, where to get the data, methods taking meteorological and seasonal variability into consideration, and insights for future studies.
Zhuang Jiang, Joel Savarino, Becky Alexander, Joseph Erbland, Jean-Luc Jaffrezo, and Lei Geng
The Cryosphere, 16, 2709–2724, https://doi.org/10.5194/tc-16-2709-2022, https://doi.org/10.5194/tc-16-2709-2022, 2022
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A record of year-round atmospheric nitrate isotopic composition along with snow nitrate isotopic data from Summit, Greenland, revealed apparent enrichments in nitrogen isotopes in snow nitrate compared to atmospheric nitrate, in addition to a relatively smaller degree of changes in oxygen isotopes. The results suggest that at this site post-depositional processing takes effect, which should be taken into account when interpreting ice-core nitrate isotope records.
Ruochong Xu, Joel A. Thornton, Ben H. Lee, Yanxu Zhang, Lyatt Jaeglé, Felipe D. Lopez-Hilfiker, Pekka Rantala, and Tuukka Petäjä
Atmos. Chem. Phys., 22, 5477–5494, https://doi.org/10.5194/acp-22-5477-2022, https://doi.org/10.5194/acp-22-5477-2022, 2022
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Monoterpenes are emitted into the atmosphere by vegetation and by the use of certain consumer products. Reactions of monoterpenes in the atmosphere lead to low-volatility products that condense to grow particulate matter or participate in new particle formation and, thus, affect air quality and climate. We use a model of atmospheric chemistry and transport to evaluate the global-scale importance of recent updates to our understanding of monoterpene chemistry in particle formation and growth.
Kathryn D. Kulju, Stephen M. McNamara, Qianjie Chen, Hannah S. Kenagy, Jacinta Edebeli, Jose D. Fuentes, Steven B. Bertman, and Kerri A. Pratt
Atmos. Chem. Phys., 22, 2553–2568, https://doi.org/10.5194/acp-22-2553-2022, https://doi.org/10.5194/acp-22-2553-2022, 2022
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N2O5 uptake by chloride-containing surfaces produces ClNO2, which photolyzes, producing NO2 and highly reactive Cl radicals that impact air quality. In the inland urban atmosphere, ClNO2 was elevated during lower air turbulence and over snow-covered ground, from snowpack ClNO2 production. N2O5 and ClNO2 levels were lowest, on average, during rainfall and fog because of scavenging, with N2O5 scavenging by fog droplets likely contributing to observed increased particulate nitrate concentrations.
Kelvin H. Bates, Daniel J. Jacob, Ke Li, Peter D. Ivatt, Mat J. Evans, Yingying Yan, and Jintai Lin
Atmos. Chem. Phys., 21, 18351–18374, https://doi.org/10.5194/acp-21-18351-2021, https://doi.org/10.5194/acp-21-18351-2021, 2021
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Simple aromatic compounds (benzene, toluene, xylene) have complex gas-phase chemistry that is inconsistently represented in atmospheric models. We compile recent experimental and theoretical insights to develop a new mechanism for gas-phase aromatic oxidation that is sufficiently compact for use in multiscale models. We compare our new mechanism to chamber experiments and other mechanisms, and implement it in a global model to quantify the impacts of aromatic oxidation on tropospheric chemistry.
Christophe Lerot, François Hendrick, Michel Van Roozendael, Leonardo M. A. Alvarado, Andreas Richter, Isabelle De Smedt, Nicolas Theys, Jonas Vlietinck, Huan Yu, Jeroen Van Gent, Trissevgeni Stavrakou, Jean-François Müller, Pieter Valks, Diego Loyola, Hitoshi Irie, Vinod Kumar, Thomas Wagner, Stefan F. Schreier, Vinayak Sinha, Ting Wang, Pucai Wang, and Christian Retscher
Atmos. Meas. Tech., 14, 7775–7807, https://doi.org/10.5194/amt-14-7775-2021, https://doi.org/10.5194/amt-14-7775-2021, 2021
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Global measurements of glyoxal tropospheric columns from the satellite instrument TROPOMI are presented. Such measurements can contribute to the estimation of atmospheric emissions of volatile organic compounds. This new glyoxal product has been fully characterized with a comprehensive error budget, with comparison with other satellite data sets as well as with validation based on independent ground-based remote sensing glyoxal observations.
Nicolas Theys, Vitali Fioletov, Can Li, Isabelle De Smedt, Christophe Lerot, Chris McLinden, Nickolay Krotkov, Debora Griffin, Lieven Clarisse, Pascal Hedelt, Diego Loyola, Thomas Wagner, Vinod Kumar, Antje Innes, Roberto Ribas, François Hendrick, Jonas Vlietinck, Hugues Brenot, and Michel Van Roozendael
Atmos. Chem. Phys., 21, 16727–16744, https://doi.org/10.5194/acp-21-16727-2021, https://doi.org/10.5194/acp-21-16727-2021, 2021
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We present a new algorithm to retrieve sulfur dioxide from space UV measurements. We apply the technique to high-resolution TROPOMI measurements and demonstrate the high sensitivity of the approach to weak SO2 emissions worldwide with an unprecedented limit of detection of 8 kt yr−1. This result has broad implications for atmospheric science studies dealing with improving emission inventories and identifying and quantifying missing sources, in the context of air quality and climate.
Hugues Brenot, Nicolas Theys, Lieven Clarisse, Jeroen van Gent, Daniel R. Hurtmans, Sophie Vandenbussche, Nikolaos Papagiannopoulos, Lucia Mona, Timo Virtanen, Andreas Uppstu, Mikhail Sofiev, Luca Bugliaro, Margarita Vázquez-Navarro, Pascal Hedelt, Michelle Maree Parks, Sara Barsotti, Mauro Coltelli, William Moreland, Simona Scollo, Giuseppe Salerno, Delia Arnold-Arias, Marcus Hirtl, Tuomas Peltonen, Juhani Lahtinen, Klaus Sievers, Florian Lipok, Rolf Rüfenacht, Alexander Haefele, Maxime Hervo, Saskia Wagenaar, Wim Som de Cerff, Jos de Laat, Arnoud Apituley, Piet Stammes, Quentin Laffineur, Andy Delcloo, Robertson Lennart, Carl-Herbert Rokitansky, Arturo Vargas, Markus Kerschbaum, Christian Resch, Raimund Zopp, Matthieu Plu, Vincent-Henri Peuch, Michel Van Roozendael, and Gerhard Wotawa
Nat. Hazards Earth Syst. Sci., 21, 3367–3405, https://doi.org/10.5194/nhess-21-3367-2021, https://doi.org/10.5194/nhess-21-3367-2021, 2021
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The purpose of the EUNADICS-AV (European Natural Airborne Disaster Information and Coordination System for Aviation) prototype early warning system (EWS) is to develop the combined use of harmonised data products from satellite, ground-based and in situ instruments to produce alerts of airborne hazards (volcanic, dust, smoke and radionuclide clouds), satisfying the requirement of aviation air traffic management (ATM) stakeholders (https://cordis.europa.eu/project/id/723986).
Arseniy Karagodin-Doyennel, Eugene Rozanov, Timofei Sukhodolov, Tatiana Egorova, Alfonso Saiz-Lopez, Carlos A. Cuevas, Rafael P. Fernandez, Tomás Sherwen, Rainer Volkamer, Theodore K. Koenig, Tanguy Giroud, and Thomas Peter
Geosci. Model Dev., 14, 6623–6645, https://doi.org/10.5194/gmd-14-6623-2021, https://doi.org/10.5194/gmd-14-6623-2021, 2021
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Here, we present the iodine chemistry module in the SOCOL-AERv2 model. The obtained iodine distribution demonstrated a good agreement when validated against other simulations and available observations. We also estimated the iodine influence on ozone in the case of present-day iodine emissions, the sensitivity of ozone to doubled iodine emissions, and when considering only organic or inorganic iodine sources. The new model can be used as a tool for further studies of iodine effects on ozone.
Xuan Wang, Daniel J. Jacob, William Downs, Shuting Zhai, Lei Zhu, Viral Shah, Christopher D. Holmes, Tomás Sherwen, Becky Alexander, Mathew J. Evans, Sebastian D. Eastham, J. Andrew Neuman, Patrick R. Veres, Theodore K. Koenig, Rainer Volkamer, L. Gregory Huey, Thomas J. Bannan, Carl J. Percival, Ben H. Lee, and Joel A. Thornton
Atmos. Chem. Phys., 21, 13973–13996, https://doi.org/10.5194/acp-21-13973-2021, https://doi.org/10.5194/acp-21-13973-2021, 2021
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Halogen radicals have a broad range of implications for tropospheric chemistry, air quality, and climate. We present a new mechanistic description and comprehensive simulation of tropospheric halogens in a global 3-D model and compare the model results with surface and aircraft measurements. We find that halogen chemistry decreases the global tropospheric burden of ozone by 11 %, NOx by 6 %, and OH by 4 %.
Andreas Tilgner, Thomas Schaefer, Becky Alexander, Mary Barth, Jeffrey L. Collett Jr., Kathleen M. Fahey, Athanasios Nenes, Havala O. T. Pye, Hartmut Herrmann, and V. Faye McNeill
Atmos. Chem. Phys., 21, 13483–13536, https://doi.org/10.5194/acp-21-13483-2021, https://doi.org/10.5194/acp-21-13483-2021, 2021
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Feedbacks of acidity and atmospheric multiphase chemistry in deliquesced particles and clouds are crucial for the tropospheric composition, depositions, climate, and human health. This review synthesizes the current scientific knowledge on these feedbacks using both inorganic and organic aqueous-phase chemistry. Finally, this review outlines atmospheric implications and highlights the need for future investigations with respect to reducing emissions of key acid precursors in a changing world.
Zhuang Jiang, Becky Alexander, Joel Savarino, Joseph Erbland, and Lei Geng
The Cryosphere, 15, 4207–4220, https://doi.org/10.5194/tc-15-4207-2021, https://doi.org/10.5194/tc-15-4207-2021, 2021
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We used a snow photochemistry model (TRANSITS) to simulate the seasonal nitrate snow profile at Summit, Greenland. Comparisons between model outputs and observations suggest that at Summit post-depositional processing is active and probably dominates the snowpack δ15N seasonality. We also used the model to assess the degree of snow nitrate loss and the consequences in its isotopes at present and in the past, which helps for quantitative interpretations of ice-core nitrate records.
Isabelle De Smedt, Gaia Pinardi, Corinne Vigouroux, Steven Compernolle, Alkis Bais, Nuria Benavent, Folkert Boersma, Ka-Lok Chan, Sebastian Donner, Kai-Uwe Eichmann, Pascal Hedelt, François Hendrick, Hitoshi Irie, Vinod Kumar, Jean-Christopher Lambert, Bavo Langerock, Christophe Lerot, Cheng Liu, Diego Loyola, Ankie Piters, Andreas Richter, Claudia Rivera Cárdenas, Fabian Romahn, Robert George Ryan, Vinayak Sinha, Nicolas Theys, Jonas Vlietinck, Thomas Wagner, Ting Wang, Huan Yu, and Michel Van Roozendael
Atmos. Chem. Phys., 21, 12561–12593, https://doi.org/10.5194/acp-21-12561-2021, https://doi.org/10.5194/acp-21-12561-2021, 2021
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This paper assess the performances of the TROPOMI formaldehyde observations compared to its predecessor OMI at different spatial and temporal scales. We also use a global network of MAX-DOAS instruments to validate both satellite datasets for a large range of HCHO columns. The precision obtained with daily TROPOMI observations is comparable to monthly OMI observations. We present clear detection of weak HCHO column enhancements related to shipping emissions in the Indian Ocean.
Claire Lamotte, Jonathan Guth, Virginie Marécal, Martin Cussac, Paul David Hamer, Nicolas Theys, and Philipp Schneider
Atmos. Chem. Phys., 21, 11379–11404, https://doi.org/10.5194/acp-21-11379-2021, https://doi.org/10.5194/acp-21-11379-2021, 2021
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Improvements are made in a global chemical transfer model by considering a new volcanic SO2 emissions inventory, with more volcanoes referenced and more information on the altitude of injection. Better constraining volcanic emissions with this inventory improves the global, but mostly local, tropospheric sulfur composition. The tropospheric sulfur budget shows a nonlinearity to the volcanic contribution, especially to the sulfate aerosol burden and sulfur wet deposition.
Johannes de Leeuw, Anja Schmidt, Claire S. Witham, Nicolas Theys, Isabelle A. Taylor, Roy G. Grainger, Richard J. Pope, Jim Haywood, Martin Osborne, and Nina I. Kristiansen
Atmos. Chem. Phys., 21, 10851–10879, https://doi.org/10.5194/acp-21-10851-2021, https://doi.org/10.5194/acp-21-10851-2021, 2021
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Using the NAME dispersion model in combination with high-resolution SO2 satellite data from TROPOMI, we investigate the dispersion of volcanic SO2 from the 2019 Raikoke eruption. NAME accurately simulates the dispersion of SO2 during the first 2–3 weeks after the eruption and illustrates the potential of using high-resolution satellite data to identify potential limitations in dispersion models, which will ultimately help to improve efforts to forecast the dispersion of volcanic clouds.
Kun Wang, Shohei Hattori, Mang Lin, Sakiko Ishino, Becky Alexander, Kazuki Kamezaki, Naohiro Yoshida, and Shichang Kang
Atmos. Chem. Phys., 21, 8357–8376, https://doi.org/10.5194/acp-21-8357-2021, https://doi.org/10.5194/acp-21-8357-2021, 2021
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Sulfate aerosols play an important climatic role and exert adverse effects on the ecological environment and human health. In this study, we present the triple oxygen isotopic composition of sulfate from the Mt. Everest region, southern Tibetan Plateau, and decipher the formation mechanisms of atmospheric sulfate in this pristine environment. The results indicate the important role of the S(IV) + O3 pathway in atmospheric sulfate formation promoted by conditions of high cloud water pH.
Eloise A. Marais, John F. Roberts, Robert G. Ryan, Henk Eskes, K. Folkert Boersma, Sungyeon Choi, Joanna Joiner, Nader Abuhassan, Alberto Redondas, Michel Grutter, Alexander Cede, Laura Gomez, and Monica Navarro-Comas
Atmos. Meas. Tech., 14, 2389–2408, https://doi.org/10.5194/amt-14-2389-2021, https://doi.org/10.5194/amt-14-2389-2021, 2021
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Nitrogen oxides in the upper troposphere have a profound influence on the global troposphere, but routine reliable observations there are exceedingly rare. We apply cloud-slicing to TROPOMI total columns of nitrogen dioxide (NO2) at high spatial resolution to derive near-global observations of NO2 in the upper troposphere and show consistency with existing datasets. These data offer tremendous potential to address knowledge gaps in this oft underappreciated portion of the atmosphere.
Christoph A. Keller, Mathew J. Evans, K. Emma Knowland, Christa A. Hasenkopf, Sruti Modekurty, Robert A. Lucchesi, Tomohiro Oda, Bruno B. Franca, Felipe C. Mandarino, M. Valeria Díaz Suárez, Robert G. Ryan, Luke H. Fakes, and Steven Pawson
Atmos. Chem. Phys., 21, 3555–3592, https://doi.org/10.5194/acp-21-3555-2021, https://doi.org/10.5194/acp-21-3555-2021, 2021
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This study combines surface observations and model simulations to quantify the impact of COVID-19 restrictions on air quality across the world. The presented methodology removes the confounding impacts of meteorology on air pollution. Our results indicate that surface concentrations of nitrogen dioxide, an important air pollutant emitted during the combustion of fossil fuels, declined by up to 60 % following the implementation of COVID-19 containment measures.
Angharad C. Stell, Luke M. Western, Tomás Sherwen, and Matthew Rigby
Atmos. Chem. Phys., 21, 1717–1736, https://doi.org/10.5194/acp-21-1717-2021, https://doi.org/10.5194/acp-21-1717-2021, 2021
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Although it is the second-most important greenhouse gas, our understanding of the atmospheric-methane budget is limited. The uncertainty highlights the need for new tools to investigate sources and sinks. Here, we use a Gaussian process emulator to efficiently approximate the response of atmospheric-methane observations to changes in the most uncertain emission or loss processes. With this new method, we rigorously quantify the sensitivity of atmospheric observations to budget uncertainties.
Mike J. Newland, Daniel J. Bryant, Rachel E. Dunmore, Thomas J. Bannan, W. Joe F. Acton, Ben Langford, James R. Hopkins, Freya A. Squires, William Dixon, William S. Drysdale, Peter D. Ivatt, Mathew J. Evans, Peter M. Edwards, Lisa K. Whalley, Dwayne E. Heard, Eloise J. Slater, Robert Woodward-Massey, Chunxiang Ye, Archit Mehra, Stephen D. Worrall, Asan Bacak, Hugh Coe, Carl J. Percival, C. Nicholas Hewitt, James D. Lee, Tianqu Cui, Jason D. Surratt, Xinming Wang, Alastair C. Lewis, Andrew R. Rickard, and Jacqueline F. Hamilton
Atmos. Chem. Phys., 21, 1613–1625, https://doi.org/10.5194/acp-21-1613-2021, https://doi.org/10.5194/acp-21-1613-2021, 2021
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We report the formation of secondary pollutants in the urban megacity of Beijing that are typically associated with remote regions such as rainforests. This is caused by extremely low levels of nitric oxide (NO), typically expected to be high in urban areas, observed in the afternoon. This work has significant implications for how we understand atmospheric chemistry in the urban environment and thus for how to implement effective policies to improve urban air quality.
Lok N. Lamsal, Nickolay A. Krotkov, Alexander Vasilkov, Sergey Marchenko, Wenhan Qin, Eun-Su Yang, Zachary Fasnacht, Joanna Joiner, Sungyeon Choi, David Haffner, William H. Swartz, Bradford Fisher, and Eric Bucsela
Atmos. Meas. Tech., 14, 455–479, https://doi.org/10.5194/amt-14-455-2021, https://doi.org/10.5194/amt-14-455-2021, 2021
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The NASA standard nitrogen dioxide (NO2) version 4.0 product for OMI Aura incorporates the most salient improvements. It represents the first global satellite trace gas retrieval with OMI–MODIS synergy accounting for surface reflectance anisotropy in cloud and NO2 retrievals. Improved spectral fitting procedures for NO2 and oxygen dimer (for cloud) retrievals and reliance on high-resolution field-of-view-specific input information for NO2 and cloud retrievals help enhance the NO2 data quality.
Gaia Pinardi, Michel Van Roozendael, François Hendrick, Nicolas Theys, Nader Abuhassan, Alkiviadis Bais, Folkert Boersma, Alexander Cede, Jihyo Chong, Sebastian Donner, Theano Drosoglou, Anatoly Dzhola, Henk Eskes, Udo Frieß, José Granville, Jay R. Herman, Robert Holla, Jari Hovila, Hitoshi Irie, Yugo Kanaya, Dimitris Karagkiozidis, Natalia Kouremeti, Jean-Christopher Lambert, Jianzhong Ma, Enno Peters, Ankie Piters, Oleg Postylyakov, Andreas Richter, Julia Remmers, Hisahiro Takashima, Martin Tiefengraber, Pieter Valks, Tim Vlemmix, Thomas Wagner, and Folkard Wittrock
Atmos. Meas. Tech., 13, 6141–6174, https://doi.org/10.5194/amt-13-6141-2020, https://doi.org/10.5194/amt-13-6141-2020, 2020
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We validate several GOME-2 and OMI tropospheric NO2 products with 23 MAX-DOAS and 16 direct sun instruments distributed worldwide, highlighting large horizontal inhomogeneities at several sites affecting the validation results. We propose a method for quantification and correction. We show the application of such correction reduces the satellite underestimation in almost all heterogeneous cases, but a negative bias remains over the MAX-DOAS and direct sun network ensemble for both satellites.
Swaleha Inamdar, Liselotte Tinel, Rosie Chance, Lucy J. Carpenter, Prabhakaran Sabu, Racheal Chacko, Sarat C. Tripathy, Anvita U. Kerkar, Alok K. Sinha, Parli Venkateswaran Bhaskar, Amit Sarkar, Rajdeep Roy, Tomás Sherwen, Carlos Cuevas, Alfonso Saiz-Lopez, Kirpa Ram, and Anoop S. Mahajan
Atmos. Chem. Phys., 20, 12093–12114, https://doi.org/10.5194/acp-20-12093-2020, https://doi.org/10.5194/acp-20-12093-2020, 2020
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Iodine chemistry is generating a lot of interest because of its impacts on the oxidising capacity of the marine boundary and depletion of ozone. However, one of the challenges has been predicting the right levels of iodine in the models, which depend on parameterisations for emissions from the sea surface. This paper discusses the different parameterisations available and compares them with observations, showing that our current knowledge is still insufficient, especially on a regional scale.
Ilias Bougoudis, Anne-Marlene Blechschmidt, Andreas Richter, Sora Seo, John Philip Burrows, Nicolas Theys, and Annette Rinke
Atmos. Chem. Phys., 20, 11869–11892, https://doi.org/10.5194/acp-20-11869-2020, https://doi.org/10.5194/acp-20-11869-2020, 2020
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A 22-year (1996 to 2017) consistent Arctic tropospheric BrO dataset derived from four satellite remote sensing instruments is presented. An increase in tropospheric BrO VCDs over this period, and especially during polar springs, can be seen. Comparisons of tropospheric BrO VCDs with first-year sea ice reveal a moderate spatial and temporal correlation between the two, suggesting that the increase in first-year sea ice in the Arctic has an impact on tropospheric BrO abundancies.
Peter D. Ivatt and Mathew J. Evans
Atmos. Chem. Phys., 20, 8063–8082, https://doi.org/10.5194/acp-20-8063-2020, https://doi.org/10.5194/acp-20-8063-2020, 2020
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We investigate the potential of using a decision tree algorithm to identify and correct the tropospheric ozone bias in a chemical transport model. We train the algorithm on 2010–2015 ground and column observation data and test the algorithm on the 2016–2017 data using the ground data as well as independent flight data. We find the algorithm is successfully able to identify and correct the bias, improving the model performance.
Katherine R. Travis, Colette L. Heald, Hannah M. Allen, Eric C. Apel, Stephen R. Arnold, Donald R. Blake, William H. Brune, Xin Chen, Róisín Commane, John D. Crounse, Bruce C. Daube, Glenn S. Diskin, James W. Elkins, Mathew J. Evans, Samuel R. Hall, Eric J. Hintsa, Rebecca S. Hornbrook, Prasad S. Kasibhatla, Michelle J. Kim, Gan Luo, Kathryn McKain, Dylan B. Millet, Fred L. Moore, Jeffrey Peischl, Thomas B. Ryerson, Tomás Sherwen, Alexander B. Thames, Kirk Ullmann, Xuan Wang, Paul O. Wennberg, Glenn M. Wolfe, and Fangqun Yu
Atmos. Chem. Phys., 20, 7753–7781, https://doi.org/10.5194/acp-20-7753-2020, https://doi.org/10.5194/acp-20-7753-2020, 2020
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Atmospheric models overestimate the rate of removal of trace gases by the hydroxyl radical (OH). This is a concern for studies of the climate and air quality impacts of human activities. Here, we evaluate the performance of a commonly used model of atmospheric chemistry against data from the NASA Atmospheric Tomography Mission (ATom) over the remote oceans where models have received little validation. The model is generally successful, suggesting that biases in OH may be a concern over land.
Marcus Hirtl, Delia Arnold, Rocio Baro, Hugues Brenot, Mauro Coltelli, Kurt Eschbacher, Helmut Hard-Stremayer, Florian Lipok, Christian Maurer, Dieter Meinhard, Lucia Mona, Marie D. Mulder, Nikolaos Papagiannopoulos, Michael Pernsteiner, Matthieu Plu, Lennart Robertson, Carl-Herbert Rokitansky, Barbara Scherllin-Pirscher, Klaus Sievers, Mikhail Sofiev, Wim Som de Cerff, Martin Steinheimer, Martin Stuefer, Nicolas Theys, Andreas Uppstu, Saskia Wagenaar, Roland Winkler, Gerhard Wotawa, Fritz Zobl, and Raimund Zopp
Nat. Hazards Earth Syst. Sci., 20, 1719–1739, https://doi.org/10.5194/nhess-20-1719-2020, https://doi.org/10.5194/nhess-20-1719-2020, 2020
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The paper summarizes the set-up and outcome of a volcanic-hazard demonstration exercise, with the goals of assessing and mitigating the impacts of volcanic ash clouds on civil and military aviation. Experts in the field simulated the sequence of procedures for an artificial eruption of the Etna volcano in Italy. The scope of the exercise ranged from the detection of the assumed event to the issuance of early warnings and optimized rerouting of flights.
Sungyeon Choi, Lok N. Lamsal, Melanie Follette-Cook, Joanna Joiner, Nickolay A. Krotkov, William H. Swartz, Kenneth E. Pickering, Christopher P. Loughner, Wyat Appel, Gabriele Pfister, Pablo E. Saide, Ronald C. Cohen, Andrew J. Weinheimer, and Jay R. Herman
Atmos. Meas. Tech., 13, 2523–2546, https://doi.org/10.5194/amt-13-2523-2020, https://doi.org/10.5194/amt-13-2523-2020, 2020
Vitali Fioletov, Chris A. McLinden, Debora Griffin, Nicolas Theys, Diego G. Loyola, Pascal Hedelt, Nickolay A. Krotkov, and Can Li
Atmos. Chem. Phys., 20, 5591–5607, https://doi.org/10.5194/acp-20-5591-2020, https://doi.org/10.5194/acp-20-5591-2020, 2020
Adrianus de Laat, Margarita Vazquez-Navarro, Nicolas Theys, and Piet Stammes
Nat. Hazards Earth Syst. Sci., 20, 1203–1217, https://doi.org/10.5194/nhess-20-1203-2020, https://doi.org/10.5194/nhess-20-1203-2020, 2020
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TROPOMI satellite measurements can accurately determine the height of thick volcanic ash clouds from a short-lived volcanic eruption of the Sinabung volcano in Indonesia. Standard geostationary satellite detection of volcanic ash was limited due to the presence of water and ice in the upper parts of volcanic ash clouds, a known issue. The TROPOMI satellite measurements do not suffer from this limitation, hence providing information where standard geostationary volcanic ash detection is limited.
Havala O. T. Pye, Athanasios Nenes, Becky Alexander, Andrew P. Ault, Mary C. Barth, Simon L. Clegg, Jeffrey L. Collett Jr., Kathleen M. Fahey, Christopher J. Hennigan, Hartmut Herrmann, Maria Kanakidou, James T. Kelly, I-Ting Ku, V. Faye McNeill, Nicole Riemer, Thomas Schaefer, Guoliang Shi, Andreas Tilgner, John T. Walker, Tao Wang, Rodney Weber, Jia Xing, Rahul A. Zaveri, and Andreas Zuend
Atmos. Chem. Phys., 20, 4809–4888, https://doi.org/10.5194/acp-20-4809-2020, https://doi.org/10.5194/acp-20-4809-2020, 2020
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Acid rain is recognized for its impacts on human health and ecosystems, and programs to mitigate these effects have had implications for atmospheric acidity. Historical measurements indicate that cloud and fog droplet acidity has changed in recent decades in response to controls on emissions from human activity, while the limited trend data for suspended particles indicate acidity may be relatively constant. This review synthesizes knowledge on the acidity of atmospheric particles and clouds.
Ryan J. Pound, Tomás Sherwen, Detlev Helmig, Lucy J. Carpenter, and Mat J. Evans
Atmos. Chem. Phys., 20, 4227–4239, https://doi.org/10.5194/acp-20-4227-2020, https://doi.org/10.5194/acp-20-4227-2020, 2020
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Ozone is an important pollutant with impacts on health and the environment. Ozone is lost to plants, land and the oceans. Loss to the ocean is slow compared to all other types of land cover and has not received as much attention. We build on previous work to more accurately model ozone loss to the ocean. We find changes in the concentration of ozone over the oceans, notably the Southern Ocean, which improves model performance.
Becky Alexander, Tomás Sherwen, Christopher D. Holmes, Jenny A. Fisher, Qianjie Chen, Mat J. Evans, and Prasad Kasibhatla
Atmos. Chem. Phys., 20, 3859–3877, https://doi.org/10.5194/acp-20-3859-2020, https://doi.org/10.5194/acp-20-3859-2020, 2020
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Nitrogen oxides are important for the formation of tropospheric oxidants and are removed from the atmosphere mainly through the formation of nitrate. We compare observations of the oxygen isotopes of nitrate with a global model to test our understanding of the chemistry nitrate formation. We use the model to quantify nitrate formation pathways in the atmosphere and identify key uncertainties and their relevance for the oxidation capacity of the atmosphere.
Sophie L. Haslett, Jonathan W. Taylor, Mathew Evans, Eleanor Morris, Bernhard Vogel, Alima Dajuma, Joel Brito, Anneke M. Batenburg, Stephan Borrmann, Johannes Schneider, Christiane Schulz, Cyrielle Denjean, Thierry Bourrianne, Peter Knippertz, Régis Dupuy, Alfons Schwarzenböck, Daniel Sauer, Cyrille Flamant, James Dorsey, Ian Crawford, and Hugh Coe
Atmos. Chem. Phys., 19, 15217–15234, https://doi.org/10.5194/acp-19-15217-2019, https://doi.org/10.5194/acp-19-15217-2019, 2019
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Three aircraft datasets from the DACCIWA campaign in summer 2016 are used here to show there is a background mass of pollution present in the lower atmosphere in southern West Africa. We suggest that this likely comes from biomass burning in central and southern Africa, which has been carried into the region over the Atlantic Ocean. This would have a negative health impact on populations living near the coast and may alter the impact of growing city emissions on cloud formation and the monsoon.
Tomás Sherwen, Rosie J. Chance, Liselotte Tinel, Daniel Ellis, Mat J. Evans, and Lucy J. Carpenter
Earth Syst. Sci. Data, 11, 1239–1262, https://doi.org/10.5194/essd-11-1239-2019, https://doi.org/10.5194/essd-11-1239-2019, 2019
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Iodine plays an important role in the Earth system, as a nutrient to the biosphere and by changing the concentrations of climate and air-quality species. However, there are uncertainties on the magnitude of iodine’s role, and a key uncertainty is our understanding of iodide in the global sea-surface. Here we take a data-driven approach using a machine learning algorithm to convert a sparse set of sea-surface iodide observations into a spatially and temporally resolved dataset for use in models.
Rachel F. Silvern, Daniel J. Jacob, Loretta J. Mickley, Melissa P. Sulprizio, Katherine R. Travis, Eloise A. Marais, Ronald C. Cohen, Joshua L. Laughner, Sungyeon Choi, Joanna Joiner, and Lok N. Lamsal
Atmos. Chem. Phys., 19, 8863–8878, https://doi.org/10.5194/acp-19-8863-2019, https://doi.org/10.5194/acp-19-8863-2019, 2019
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The US EPA reports a steady decrease in nitrogen oxide (NOx) emissions from fuel combustion over the 2005–2017 period, while satellite observations show a leveling off after 2009, suggesting emission reductions and related air quality gains have halted. We show the sustained decrease in NOx emissions is in fact consistent with observed trends in surface NO2 and ozone concentrations and that the flattening of the satellite trend reflects a growing influence from the non-anthropogenic background.
Lei Zhu, Daniel J. Jacob, Sebastian D. Eastham, Melissa P. Sulprizio, Xuan Wang, Tomás Sherwen, Mat J. Evans, Qianjie Chen, Becky Alexander, Theodore K. Koenig, Rainer Volkamer, L. Gregory Huey, Michael Le Breton, Thomas J. Bannan, and Carl J. Percival
Atmos. Chem. Phys., 19, 6497–6507, https://doi.org/10.5194/acp-19-6497-2019, https://doi.org/10.5194/acp-19-6497-2019, 2019
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We quantify the effect of sea salt aerosol on tropospheric bromine chemistry with a new mechanistic description of the halogen chemistry in a global atmospheric chemistry model. For the first time, we are able to reproduce the observed levels of bromide activation from the sea salt aerosol in a manner consistent with bromine oxide radical measured from various platforms. Sea salt aerosol plays a far more complex role in global tropospheric chemistry than previously recognized.
Jingyuan Shao, Qianjie Chen, Yuxuan Wang, Xiao Lu, Pengzhen He, Yele Sun, Viral Shah, Randall V. Martin, Sajeev Philip, Shaojie Song, Yue Zhao, Zhouqing Xie, Lin Zhang, and Becky Alexander
Atmos. Chem. Phys., 19, 6107–6123, https://doi.org/10.5194/acp-19-6107-2019, https://doi.org/10.5194/acp-19-6107-2019, 2019
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Sulfate is a key species contributing to particle formation and growth during wintertime Chinese haze events. This study combines observations and modeling of oxygen isotope signatures in sulfate aerosol to investigate its formation mechanisms, with a focus on heterogeneous production on aerosol surface via H2O2, O3, and NO2 and trace metal catalyzed oxidation. Contributions from different formation pathways are presented.
Yang Wang, Steffen Dörner, Sebastian Donner, Sebastian Böhnke, Isabelle De Smedt, Russell R. Dickerson, Zipeng Dong, Hao He, Zhanqing Li, Zhengqiang Li, Donghui Li, Dong Liu, Xinrong Ren, Nicolas Theys, Yuying Wang, Yang Wang, Zhenzhu Wang, Hua Xu, Jiwei Xu, and Thomas Wagner
Atmos. Chem. Phys., 19, 5417–5449, https://doi.org/10.5194/acp-19-5417-2019, https://doi.org/10.5194/acp-19-5417-2019, 2019
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A MAX-DOAS instrument was operated to derive tropospheric vertical profiles of NO2, SO2, HONO, HCHO, CHOCHO and aerosols in the central western North China Plain in May and June 2016. The MAX-DOAS results are verified by comparisons with a collocated Raman lidar, overpass aircraft measurements, a sun photometer and in situ measurements. The contributions of regional transports and local emissions to the pollutants are evaluated based on case studies and statistic analysis.
Elisa Carboni, Tamsin A. Mather, Anja Schmidt, Roy G. Grainger, Melissa A. Pfeffer, Iolanda Ialongo, and Nicolas Theys
Atmos. Chem. Phys., 19, 4851–4862, https://doi.org/10.5194/acp-19-4851-2019, https://doi.org/10.5194/acp-19-4851-2019, 2019
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The 2014–2015 Holuhraun eruption was the largest in Iceland for 200 years, emitting huge quantities of gas into the troposphere, at times overwhelming European anthropogenic emissions. Infrared Atmospheric sounding Interferometer data are used to derive the first time series of daily sulfur dioxide mass and vertical distribution over the eruption period. A scheme is used to estimate sulfur dioxide fluxes, the total erupted mass, and how long the sulfur dioxide remains in the atmosphere.
Raid M. Suleiman, Kelly Chance, Xiong Liu, Gonzalo González Abad, Thomas P. Kurosu, Francois Hendrick, and Nicolas Theys
Atmos. Meas. Tech., 12, 2067–2084, https://doi.org/10.5194/amt-12-2067-2019, https://doi.org/10.5194/amt-12-2067-2019, 2019
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This paper presents the retrieval algorithm for the operational OMBRO data product and shows comparisons with correlative measurements and retrieval results. We highlight the physics of the retrieval. We compare the OMBRO products with other satellite and in situ measurements of BrO and illustrate the quality of the product on a global scale. We study OMBRO enhancements in volcanic plumes and over salt lakes. We also discuss the shortcomings and future updates of the OMBRO product.
Christoph A. Keller and Mat J. Evans
Geosci. Model Dev., 12, 1209–1225, https://doi.org/10.5194/gmd-12-1209-2019, https://doi.org/10.5194/gmd-12-1209-2019, 2019
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Computer simulations of atmospheric chemistry are a central tool to study the impact of air pollutants on the environment. These models are highly complex and require a lot of computing resources. In this study we show that machine learning can be used to predict air pollution with an accuracy that is comparable to the traditional, computationally expensive method. Such a machine-learning-based model has the potential to be orders of magnitude faster.
Xuan Wang, Daniel J. Jacob, Sebastian D. Eastham, Melissa P. Sulprizio, Lei Zhu, Qianjie Chen, Becky Alexander, Tomás Sherwen, Mathew J. Evans, Ben H. Lee, Jessica D. Haskins, Felipe D. Lopez-Hilfiker, Joel A. Thornton, Gregory L. Huey, and Hong Liao
Atmos. Chem. Phys., 19, 3981–4003, https://doi.org/10.5194/acp-19-3981-2019, https://doi.org/10.5194/acp-19-3981-2019, 2019
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Chlorine radicals have a broad range of implications for tropospheric chemistry, air quality, and climate. We present a comprehensive simulation of tropospheric chlorine in a global 3-D model, which includes explicit accounting of chloride mobilization from sea salt aerosol. We find the chlorine chemistry contributes 1.0 % of the global oxidation of methane and decreases global burdens of tropospheric ozone by 7 % and OH by 3 % through the associated bromine radical chemistry.
Alba Badia, Claire E. Reeves, Alex R. Baker, Alfonso Saiz-Lopez, Rainer Volkamer, Theodore K. Koenig, Eric C. Apel, Rebecca S. Hornbrook, Lucy J. Carpenter, Stephen J. Andrews, Tomás Sherwen, and Roland von Glasow
Atmos. Chem. Phys., 19, 3161–3189, https://doi.org/10.5194/acp-19-3161-2019, https://doi.org/10.5194/acp-19-3161-2019, 2019
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The oceans have an impact on the composition and reactivity of the troposphere through the emission of gases and particles. Thus, a quantitative understanding of the marine atmosphere is crucial to examine the oxidative capacity and climate forcing. This study investigates the impact of halogens in the tropical troposphere and explores the sensitivity of this to uncertainties in the fluxes and their chemical processing. Our modelled tropospheric Ox loss due to halogens ranges from 20 % to 60 %.
Kate R. Smith, Peter M. Edwards, Peter D. Ivatt, James D. Lee, Freya Squires, Chengliang Dai, Richard E. Peltier, Mat J. Evans, Yele Sun, and Alastair C. Lewis
Atmos. Meas. Tech., 12, 1325–1336, https://doi.org/10.5194/amt-12-1325-2019, https://doi.org/10.5194/amt-12-1325-2019, 2019
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Clusters of low-cost, low-power atmospheric gas sensors were built into a sensor instrument to monitor NO2 and O3 in Beijing, alongside reference instruments, aiming to improve the reliability of sensor measurements. Clustering identical sensors and using the median sensor signal was used to minimize drift over short and medium timescales. Three different machine learning techniques were used for all the sensor data in an attempt to correct for cross-interferences, which worked to some degree.
Federica Pacifico, Claire Delon, Corinne Jambert, Pierre Durand, Eleanor Morris, Mat J. Evans, Fabienne Lohou, Solène Derrien, Venance H. E. Donnou, Arnaud V. Houeto, Irene Reinares Martínez, and Pierre-Etienne Brilouet
Atmos. Chem. Phys., 19, 2299–2325, https://doi.org/10.5194/acp-19-2299-2019, https://doi.org/10.5194/acp-19-2299-2019, 2019
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Biogenic fluxes from soil at a local and regional scale are crucial to study air pollution and climate. Here we present field measurements of soil fluxes of nitric oxide (NO) and ammonia (NH3) observed over four different land cover types, i.e. bare soil, grassland, maize field, and forest, at an inland rural site in Benin, West Africa, during the DACCIWA field campaign in
June and July 2016.
Ting Wang, Pucai Wang, Nicolas Theys, Dan Tong, François Hendrick, Qiang Zhang, and Michel Van Roozendael
Atmos. Chem. Phys., 18, 18063–18078, https://doi.org/10.5194/acp-18-18063-2018, https://doi.org/10.5194/acp-18-18063-2018, 2018
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In the last decade, four temporal regimes of SO2 in China have been identified. After an initial rise, SO2 undergoes two sharp drops in 2007–2008 and 2014–2016, during which 5-year rebounding is sustained. Different mechanisms are tied to North and South China. The industrial emission is responsible for SO2 variation in North China, while in South China the meteorological conditions make a large contribution. The result is crucial to the understanding of SO2 changes and future polices.
Eloise A. Marais, Daniel J. Jacob, Sungyeon Choi, Joanna Joiner, Maria Belmonte-Rivas, Ronald C. Cohen, Steffen Beirle, Lee T. Murray, Luke D. Schiferl, Viral Shah, and Lyatt Jaeglé
Atmos. Chem. Phys., 18, 17017–17027, https://doi.org/10.5194/acp-18-17017-2018, https://doi.org/10.5194/acp-18-17017-2018, 2018
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We intercompare two new products of global upper tropospheric nitrogen dioxide (NO2) retrieved from the Ozone Monitoring Instrument (OMI). We evaluate these products with aircraft observations from NASA DC8 aircraft campaigns and interpret the useful information these products can provide about nitrogen oxides (NOx) in the global upper troposphere using the GEOS-Chem chemical transport model.
Fei Liu, Sungyeon Choi, Can Li, Vitali E. Fioletov, Chris A. McLinden, Joanna Joiner, Nickolay A. Krotkov, Huisheng Bian, Greet Janssens-Maenhout, Anton S. Darmenov, and Arlindo M. da Silva
Atmos. Chem. Phys., 18, 16571–16586, https://doi.org/10.5194/acp-18-16571-2018, https://doi.org/10.5194/acp-18-16571-2018, 2018
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Sulfur dioxide measurements from space have been used to detect emissions from large sources. We developed a new emission inventory by combining the satellite-based emission estimates and the conventional bottom-up inventory for smaller sources. The new inventory improves the model agreement with in situ observations and offers the possibility of rapid updates to emissions.
Jiayue Huang, Lyatt Jaeglé, and Viral Shah
Atmos. Chem. Phys., 18, 16253–16269, https://doi.org/10.5194/acp-18-16253-2018, https://doi.org/10.5194/acp-18-16253-2018, 2018
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The contribution of blowing snow and frost flower as sources of sea salt aerosols (SSA) over polar regions remains uncertain, despite its potentially important role in polar climate and chemistry. Using chemical transport models and satellite observations, we find that blowing snow emissions are the dominant source of SSA over sea ice during the cold season. We infer a monthly snow salinity on first-year sea ice that decreases from fall–spring, minimizing the model discrepancy to within 10 %.
Lu Hu, Christoph A. Keller, Michael S. Long, Tomás Sherwen, Benjamin Auer, Arlindo Da Silva, Jon E. Nielsen, Steven Pawson, Matthew A. Thompson, Atanas L. Trayanov, Katherine R. Travis, Stuart K. Grange, Mat J. Evans, and Daniel J. Jacob
Geosci. Model Dev., 11, 4603–4620, https://doi.org/10.5194/gmd-11-4603-2018, https://doi.org/10.5194/gmd-11-4603-2018, 2018
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We present a full-year online global simulation of tropospheric chemistry at 12.5 km resolution. To the best of our knowledge, such a resolution in a state-of-the-science global simulation of tropospheric chemistry is unprecedented. This simulation will serve as the Nature Run for observing system simulation experiments to support the future geostationary satellite constellation for tropospheric chemistry, and can also be used for various air quality applications.
Qianjie Chen, Tomás Sherwen, Mathew Evans, and Becky Alexander
Atmos. Chem. Phys., 18, 13617–13637, https://doi.org/10.5194/acp-18-13617-2018, https://doi.org/10.5194/acp-18-13617-2018, 2018
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Uncertainty in the natural tropospheric sulfur cycle represents the largest source of uncertainty in radiative forcing estimates of sulfate aerosol. This study investigates the natural sulfur cycle in the marine troposphere using the GEOS-Chem model. We found that BrO is important for DMS oxidation and multiphase chemistry is important for MSA production and loss, which have implications for the yield of SO2 and MSA from DMS oxidation and the radiative effect of DMS-derived sulfate aerosol.
Prasad Kasibhatla, Tomás Sherwen, Mathew J. Evans, Lucy J. Carpenter, Chris Reed, Becky Alexander, Qianjie Chen, Melissa P. Sulprizio, James D. Lee, Katie A. Read, William Bloss, Leigh R. Crilley, William C. Keene, Alexander A. P. Pszenny, and Alma Hodzic
Atmos. Chem. Phys., 18, 11185–11203, https://doi.org/10.5194/acp-18-11185-2018, https://doi.org/10.5194/acp-18-11185-2018, 2018
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Recent measurements of NOx and HONO suggest that photolysis of particulate nitrate in sea-salt aerosols is important in terms of marine boundary layer oxidant chemistry. We present the first global-scale assessment of the significance of this new chemical pathway for NOx, O3, and OH in the marine boundary layer. We also present a preliminary assessment of the potential impact of photolysis of particulate nitrate associated with other aerosol types on continental boundary layer chemistry.
Mike J. Newland, Andrew R. Rickard, Tomás Sherwen, Mathew J. Evans, Luc Vereecken, Amalia Muñoz, Milagros Ródenas, and William J. Bloss
Atmos. Chem. Phys., 18, 6095–6120, https://doi.org/10.5194/acp-18-6095-2018, https://doi.org/10.5194/acp-18-6095-2018, 2018
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Stabilised Criegee intermediates (SCIs) are formed in the reaction of alkenes with ozone, both of which are ubiquitous throughout the troposphere. We determine the fate and global distribution of SCI from monoterpene ozonolysis. One major fate of SCI is reaction with H2O, but for a fraction of SCIs, unimolecular reactions dominate. Concentrations of SCIs are high enough regionally to play a key role in the conversion of sulfur dioxide to aerosol, affecting air quality and climate.
Isabelle De Smedt, Nicolas Theys, Huan Yu, Thomas Danckaert, Christophe Lerot, Steven Compernolle, Michel Van Roozendael, Andreas Richter, Andreas Hilboll, Enno Peters, Mattia Pedergnana, Diego Loyola, Steffen Beirle, Thomas Wagner, Henk Eskes, Jos van Geffen, Klaas Folkert Boersma, and Pepijn Veefkind
Atmos. Meas. Tech., 11, 2395–2426, https://doi.org/10.5194/amt-11-2395-2018, https://doi.org/10.5194/amt-11-2395-2018, 2018
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This paper introduces the formaldehyde (HCHO) tropospheric vertical column retrieval algorithm implemented in the TROPOMI/Sentinel-5 Precursor operational processor, and comprehensively describes its various retrieval steps. Furthermore, algorithmic improvements developed in the framework of the EU FP7-project QA4ECV are described for future updates of the processor. Detailed error estimates are discussed in the light of Copernicus user requirements and needs for validation are highlighted.
Pengzhen He, Becky Alexander, Lei Geng, Xiyuan Chi, Shidong Fan, Haicong Zhan, Hui Kang, Guangjie Zheng, Yafang Cheng, Hang Su, Cheng Liu, and Zhouqing Xie
Atmos. Chem. Phys., 18, 5515–5528, https://doi.org/10.5194/acp-18-5515-2018, https://doi.org/10.5194/acp-18-5515-2018, 2018
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We use observations of the oxygen isotopic composition of sulfate aerosol as a fingerprint to quantify various sulfate formation mechanisms during pollution events in Beijing, China. We found that heterogeneous reactions on aerosols dominated sulfate production in general; however, in-cloud reactions would dominate haze sulfate production when cloud liquid water content was high. The findings also suggest the heterogeneity of aerosol acidity should be parameterized in models.
Maria Elissavet Koukouli, Nicolas Theys, Jieying Ding, Irene Zyrichidou, Bas Mijling, Dimitrios Balis, and Ronald Johannes van der A
Atmos. Meas. Tech., 11, 1817–1832, https://doi.org/10.5194/amt-11-1817-2018, https://doi.org/10.5194/amt-11-1817-2018, 2018
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Within the framework of the EU FP7 project MarcoPolo (Monitoring and Assessment of Regional air quality in China using space Observations), a new SO2 emission inventory over China was calculated using the CHIMERE CTM simulations, 10 years of OMI/Aura total SO2 columns and the bottom-up Multi-resolution Emission Inventory for China (MEIC v1.2).
Daniel Stone, Tomás Sherwen, Mathew J. Evans, Stewart Vaughan, Trevor Ingham, Lisa K. Whalley, Peter M. Edwards, Katie A. Read, James D. Lee, Sarah J. Moller, Lucy J. Carpenter, Alastair C. Lewis, and Dwayne E. Heard
Atmos. Chem. Phys., 18, 3541–3561, https://doi.org/10.5194/acp-18-3541-2018, https://doi.org/10.5194/acp-18-3541-2018, 2018
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Halogen chemistry in the troposphere impacts oxidising capacity, but model studies assessing the nature of these impacts can vary according to the model framework used. In this work we present simulations of OH and HO2 radicals using both box and global model frameworks, and compare to observations made at the Cape Verde Atmospheric Observatory. We highlight, and rationalise, differences between the model frameworks.
Theodore K. Koenig, Rainer Volkamer, Sunil Baidar, Barbara Dix, Siyuan Wang, Daniel C. Anderson, Ross J. Salawitch, Pamela A. Wales, Carlos A. Cuevas, Rafael P. Fernandez, Alfonso Saiz-Lopez, Mathew J. Evans, Tomás Sherwen, Daniel J. Jacob, Johan Schmidt, Douglas Kinnison, Jean-François Lamarque, Eric C. Apel, James C. Bresch, Teresa Campos, Frank M. Flocke, Samuel R. Hall, Shawn B. Honomichl, Rebecca Hornbrook, Jørgen B. Jensen, Richard Lueb, Denise D. Montzka, Laura L. Pan, J. Michael Reeves, Sue M. Schauffler, Kirk Ullmann, Andrew J. Weinheimer, Elliot L. Atlas, Valeria Donets, Maria A. Navarro, Daniel Riemer, Nicola J. Blake, Dexian Chen, L. Gregory Huey, David J. Tanner, Thomas F. Hanisco, and Glenn M. Wolfe
Atmos. Chem. Phys., 17, 15245–15270, https://doi.org/10.5194/acp-17-15245-2017, https://doi.org/10.5194/acp-17-15245-2017, 2017
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Tropospheric inorganic bromine (BrO and Bry) shows a C-shaped profile over the tropical western Pacific Ocean, and supports previous speculation that marine convection is a source for inorganic bromine from sea salt to the upper troposphere. The Bry profile in the tropical tropopause layer (TTL) is complex, suggesting that the total Bry budget in the TTL is not closed without considering aerosol bromide. The implications for atmospheric composition and bromine sources are discussed.
Ben Newsome and Mat Evans
Atmos. Chem. Phys., 17, 14333–14352, https://doi.org/10.5194/acp-17-14333-2017, https://doi.org/10.5194/acp-17-14333-2017, 2017
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We explore the uncertainty in the predictions of a chemical transport model (GEOS-Chem) from uncertainty in 60 inorganic rate constants and photolysis rates. We find uncertainty in the global mean ozone burden of 10 %, in global mean OH of 16 %, methane lifetimes of 16 %, and tropospheric ozone radiative forcings of 13 %. Reductions in the uncertainty of rate constants of these simple reactions would reduce uncertainty in our understanding of atmospheric composition.
Peter M. Edwards and Mathew J. Evans
Atmos. Chem. Phys., 17, 13669–13680, https://doi.org/10.5194/acp-17-13669-2017, https://doi.org/10.5194/acp-17-13669-2017, 2017
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Understanding tropospheric ozone chemistry has been at the centre of the field of atmospheric chemistry for the last 30 years. However, our conceptual approach to diagnosing ozone production in global models has not advanced in this time. Our work presents a new and powerful approach for diagnosing tropospheric ozone production, providing a significant enhancement in our ability to understand the processes controlling ozone and how we can validate our assessment of these processes.
Peter Knippertz, Andreas H. Fink, Adrien Deroubaix, Eleanor Morris, Flore Tocquer, Mat J. Evans, Cyrille Flamant, Marco Gaetani, Christophe Lavaysse, Celine Mari, John H. Marsham, Rémi Meynadier, Abalo Affo-Dogo, Titike Bahaga, Fabien Brosse, Konrad Deetz, Ridha Guebsi, Issaou Latifou, Marlon Maranan, Philip D. Rosenberg, and Andreas Schlueter
Atmos. Chem. Phys., 17, 10893–10918, https://doi.org/10.5194/acp-17-10893-2017, https://doi.org/10.5194/acp-17-10893-2017, 2017
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In June–July 2016 DACCIWA (Dynamics–Aerosol–Chemistry–Cloud Interactions in West Africa), a large, EU-funded European–African project, organised an international field campaign in densely populated southern West Africa, including measurements from ground sites, research aircraft, weather balloons and urban sites. This paper gives an overview of the atmospheric evolution during this period focusing on meteorological (precipitation, cloudiness, winds) and composition (gases, particles) aspects.
Viral Shah and Lyatt Jaeglé
Atmos. Chem. Phys., 17, 8999–9017, https://doi.org/10.5194/acp-17-8999-2017, https://doi.org/10.5194/acp-17-8999-2017, 2017
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We use a model of mercury chemistry and transport in the atmosphere, along with ground- and aircraft-based mercury observations, to learn that oxidized mercury chemically produced in the free troposphere descends in the subtropical anticyclones and makes up much of the mercury depositing to the Earth's surface. Our findings imply that mercury chemistry in the free troposphere and transport in the subtropics are important links between global emissions and surface deposition of mercury.
Johannes Bieser, Franz Slemr, Jesse Ambrose, Carl Brenninkmeijer, Steve Brooks, Ashu Dastoor, Francesco DeSimone, Ralf Ebinghaus, Christian N. Gencarelli, Beate Geyer, Lynne E. Gratz, Ian M. Hedgecock, Daniel Jaffe, Paul Kelley, Che-Jen Lin, Lyatt Jaegle, Volker Matthias, Andrei Ryjkov, Noelle E. Selin, Shaojie Song, Oleg Travnikov, Andreas Weigelt, Winston Luke, Xinrong Ren, Andreas Zahn, Xin Yang, Yun Zhu, and Nicola Pirrone
Atmos. Chem. Phys., 17, 6925–6955, https://doi.org/10.5194/acp-17-6925-2017, https://doi.org/10.5194/acp-17-6925-2017, 2017
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We conducted a multi model study to investigate our ability to reproduce the vertical distribution of mercury in the atmosphere. For this, we used observational data from over 40 aircraft flights in EU and US. We compared observations to the results of seven chemistry transport models and found that the models are able to reproduce vertical gradients of total and elemental Hg. Finally, we found that different chemical reactions seem responsible for the oxidation of Hg depending on altitude.
Yang Wang, Steffen Beirle, Johannes Lampel, Mariliza Koukouli, Isabelle De Smedt, Nicolas Theys, Ang Li, Dexia Wu, Pinhua Xie, Cheng Liu, Michel Van Roozendael, Trissevgeni Stavrakou, Jean-François Müller, and Thomas Wagner
Atmos. Chem. Phys., 17, 5007–5033, https://doi.org/10.5194/acp-17-5007-2017, https://doi.org/10.5194/acp-17-5007-2017, 2017
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A long-term MAX-DOAS measurement from 2011 to 2014 was operated in Wuxi, part of the most industrialized area of the Yangtze River delta region of China. The tropospheric VCDs and vertical profiles of NO2, SO2 and HCHO derived from the MAX-DOAS are used to validate the products derived from OMI and GOME-2A/B by different scientific teams (daily- and bimonthly-averaged data). We investigate the effects of clouds, aerosols and a priori profile shapes on satellite retrievals of tropospheric VCDs.
Anja Schönhardt, Andreas Richter, Nicolas Theys, and John P. Burrows
Atmos. Chem. Phys., 17, 4857–4870, https://doi.org/10.5194/acp-17-4857-2017, https://doi.org/10.5194/acp-17-4857-2017, 2017
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Iodine monoxide, IO, is observed in satellite measurements following the eruption of the Kasatochi volcano, Alaska, in August 2008. Large IO columns are detected by SCIAMACHY on ENVISAT and by GOME-2 on MetOp-A for several days. IO amounts are approximately 1 order of magnitude smaller than those of BrO. Details in the spatial distributions differ between IO, BrO and sulfur dioxide, SO2. The total mass of IO in the volcanic plume is determined to be on the order of 10 Mg.
Chris Reed, Mathew J. Evans, Leigh R. Crilley, William J. Bloss, Tomás Sherwen, Katie A. Read, James D. Lee, and Lucy J. Carpenter
Atmos. Chem. Phys., 17, 4081–4092, https://doi.org/10.5194/acp-17-4081-2017, https://doi.org/10.5194/acp-17-4081-2017, 2017
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The source of ozone-depleting compounds in the remote troposphere has been thought to be long-range transport of secondary pollutants such as organic nitrates. Processing of organic nitrates to nitric acid and subsequent deposition on surfaces in the atmosphere was thought to remove these nitrates from the ozone–NOx–HOx cycle. We found through observation of NOx in the remote tropical troposphere at the Cape Verde Observatory that surface nitrates can be released back into the atmosphere.
Jiayue Huang and Lyatt Jaeglé
Atmos. Chem. Phys., 17, 3699–3712, https://doi.org/10.5194/acp-17-3699-2017, https://doi.org/10.5194/acp-17-3699-2017, 2017
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The emissions and distribution of wintertime sea salt aerosol (SSA) are poorly constrained in polar regions, despite their potentially significant roles in halogen release, cloud formation and climate. We implement a blowing snow and a frost flower emission scheme in the model, and find that inclusion of blowing snow is necessary to simulate the observed winter and spring SSA levels. We estimate that inclusion of blowing snow increases submicron SSA emissions by factors of 2–3 in polar regions.
Ronald J. van der A, Bas Mijling, Jieying Ding, Maria Elissavet Koukouli, Fei Liu, Qing Li, Huiqin Mao, and Nicolas Theys
Atmos. Chem. Phys., 17, 1775–1789, https://doi.org/10.5194/acp-17-1775-2017, https://doi.org/10.5194/acp-17-1775-2017, 2017
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The SO2 concentrations and NOx emissions over China derived from satellite observations are compared with the national fossil fuel consumption and air quality regulations. It is shown that not only NO2 concentrations but also NOx emissions in all Chinese provinces decreased in the last 2 years. We conclude that without the air quality regulations the SO2 concentrations would be about 2.5 times higher and the NO2 concentrations would be at least 25 % higher than they are today in China.
Tomás Sherwen, Mat J. Evans, Lucy J. Carpenter, Johan A. Schmidt, and Loretta J. Mickley
Atmos. Chem. Phys., 17, 1557–1569, https://doi.org/10.5194/acp-17-1557-2017, https://doi.org/10.5194/acp-17-1557-2017, 2017
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We model pre-industrial to present day changes using the GEOS-Chem global chemical transport model with halogens (Cl, Br, I). The model better captures pre-industrial O3 observations with halogens included. Halogens buffer the tropospheric forcing of O3 (RFTO3) from pre-industrial to present day, reducing RFTO3 by 0.087 Wm−2. This reduction is greater than that from halogens on stratospheric O3 (−0.05 Wm−2). This suggests that models that do not include halogens will overestimate RFTO3by ~ 25%.
Nicolas Theys, Isabelle De Smedt, Huan Yu, Thomas Danckaert, Jeroen van Gent, Christoph Hörmann, Thomas Wagner, Pascal Hedelt, Heiko Bauer, Fabian Romahn, Mattia Pedergnana, Diego Loyola, and Michel Van Roozendael
Atmos. Meas. Tech., 10, 119–153, https://doi.org/10.5194/amt-10-119-2017, https://doi.org/10.5194/amt-10-119-2017, 2017
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This paper provides a thorough description of the algorithm to retrieve SO2 columns from TROPOMI/Sentinel-5 Precursor measurements. The different algorithmic steps including error analysis are detailed. Scientific verification of the algorithm and validation needs are also discussed.
Maria Zatko, Joseph Erbland, Joel Savarino, Lei Geng, Lauren Easley, Andrew Schauer, Timothy Bates, Patricia K. Quinn, Bonnie Light, David Morison, Hans D. Osthoff, Seth Lyman, William Neff, Bin Yuan, and Becky Alexander
Atmos. Chem. Phys., 16, 13837–13851, https://doi.org/10.5194/acp-16-13837-2016, https://doi.org/10.5194/acp-16-13837-2016, 2016
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This manuscript presents chemical and optical observations collected in the air and snow during UBWOS2014 in eastern Utah. These observations are used to calculate fluxes of reactive nitrogen associated with snow nitrate photolysis. Snow-sourced reactive nitrogen fluxes are compared to reactive nitrogen emission inventories to find that snow-sourced reactive nitrogen is a minor contributor to the reactive nitrogen budget, and thus wintertime ground-level ozone formation, in the Uintah Basin.
Tomás Sherwen, Johan A. Schmidt, Mat J. Evans, Lucy J. Carpenter, Katja Großmann, Sebastian D. Eastham, Daniel J. Jacob, Barbara Dix, Theodore K. Koenig, Roman Sinreich, Ivan Ortega, Rainer Volkamer, Alfonso Saiz-Lopez, Cristina Prados-Roman, Anoop S. Mahajan, and Carlos Ordóñez
Atmos. Chem. Phys., 16, 12239–12271, https://doi.org/10.5194/acp-16-12239-2016, https://doi.org/10.5194/acp-16-12239-2016, 2016
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We present a simulation of tropospheric Cl, Br, I chemistry within the GEOS-Chem CTM. We find a decrease in tropospheric ozone burden of 18.6 % and a 8.2 % decrease in global mean OH concentrations. Cl oxidation of some VOCs range from 15 to 27 % of the total loss. Bromine plays a small role in oxidising oVOCs. Surface ozone, ozone sondes, and methane lifetime are in general improved by the inclusion of halogens. We argue that simulated bromine and chlorine represent a lower limit.
Vitali E. Fioletov, Chris A. McLinden, Nickolay Krotkov, Can Li, Joanna Joiner, Nicolas Theys, Simon Carn, and Mike D. Moran
Atmos. Chem. Phys., 16, 11497–11519, https://doi.org/10.5194/acp-16-11497-2016, https://doi.org/10.5194/acp-16-11497-2016, 2016
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We introduce the first space-based catalogue of SO2 emission sources seen by OMI. The inventory contains about 500 sources. They account for about a half of all SO2 emissions; the remaining half is likely related to sources emitting less than 30 kt yr−1 and not detected by OMI. The sources are grouped by type (volcanoes, power plants, oil- and gas-related sources, and smelters) and country. The catalogue presented herein can be used for verification of available SO2 emission inventories.
Qianjie Chen, Lei Geng, Johan A. Schmidt, Zhouqing Xie, Hui Kang, Jordi Dachs, Jihong Cole-Dai, Andrew J. Schauer, Madeline G. Camp, and Becky Alexander
Atmos. Chem. Phys., 16, 11433–11450, https://doi.org/10.5194/acp-16-11433-2016, https://doi.org/10.5194/acp-16-11433-2016, 2016
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The formation mechanisms of sulfate in the marine boundary layer are not well understood, which could result in large uncertainties in aerosol radiative forcing. We measure the oxygen isotopic composition (Δ17O) of sulfate collected in the MBL and analyze with a global transport model. Our results suggest that 33–50 % of MBL sulfate is formed via oxidation of S(IV) by hypohalous acids HOBr / HOCl in the aqueous phase, and the daily-mean HOBr/HOCl concentrations are on the order of 0.01–0.1 ppt.
Marie Boichu, Isabelle Chiapello, Colette Brogniez, Jean-Christophe Péré, Francois Thieuleux, Benjamin Torres, Luc Blarel, Augustin Mortier, Thierry Podvin, Philippe Goloub, Nathalie Söhne, Lieven Clarisse, Sophie Bauduin, François Hendrick, Nicolas Theys, Michel Van Roozendael, and Didier Tanré
Atmos. Chem. Phys., 16, 10831–10845, https://doi.org/10.5194/acp-16-10831-2016, https://doi.org/10.5194/acp-16-10831-2016, 2016
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Bárðarbunga eruption emitted huge amounts of sulfur into the lower troposphere causing an unprecedented air pollution in the modern era. A wealth of remote sensing and in situ data allows us to jointly analyse the dynamics of volcanic SO2 and sulfate aerosols. Based on this panel of observations, success and challenges in simulating such volcanogenic long-range pollution events are exposed, focusing on the boundary layer dynamics.
Birthe Marie Steensen, Michael Schulz, Nicolas Theys, and Hilde Fagerli
Atmos. Chem. Phys., 16, 9745–9760, https://doi.org/10.5194/acp-16-9745-2016, https://doi.org/10.5194/acp-16-9745-2016, 2016
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The Bardarbunga volcanic fissure during the second half of 2014 caused large amounts of SO2 emission. The paper studies the effects of this increase in pollution levels over Europe during the first 3 months of the eruption with a dispersion model. The model results are compared to satellite and surface concentration observations. The biggest differences are found in Iceland and on the coast of northern Norway. For the average pollution levels over Europe, Iceland is located too far away.
Dene R. Bowdalo, Mathew J. Evans, and Eric D. Sofen
Atmos. Chem. Phys., 16, 8295–8308, https://doi.org/10.5194/acp-16-8295-2016, https://doi.org/10.5194/acp-16-8295-2016, 2016
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We introduce a new methodology for the assessment of atmospheric models with observations. We apply a spectral analysis methodology to hourly ozone observations and the equivalent model output. The spectrally transformed observational data show significant peaks on daily and annual timescales. Comparison between the amplitude and phase of these peaks introduces a new comparison methodology between model and measurements. We find the model shows significant biases on an annual timescale.
Alicia Gressent, Bastien Sauvage, Daniel Cariolle, Mathew Evans, Maud Leriche, Céline Mari, and Valérie Thouret
Atmos. Chem. Phys., 16, 5867–5889, https://doi.org/10.5194/acp-16-5867-2016, https://doi.org/10.5194/acp-16-5867-2016, 2016
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In chemical transport models, NOx emitted by lightning (LNOx) is instantaneously diluted into the grid. A plume-in-grid parameterization to account for the sub-grid chemistry of LNOx is presented. This approach was implemented into the GEOS-Chem model and leads to a relative increase of NOx and O3 (18 % and 2 %, respectively, in July) on a large scale downwind of lightning emissions and a relative decrease (25 % and 8 %, respectively, over central Africa in July) over the regions of emissions.
Dimitris Balis, Maria-Elissavet Koukouli, Nikolaos Siomos, Spyridon Dimopoulos, Lucia Mona, Gelsomina Pappalardo, Franco Marenco, Lieven Clarisse, Lucy J. Ventress, Elisa Carboni, Roy G. Grainger, Ping Wang, Gijsbert Tilstra, Ronald van der A, Nicolas Theys, and Claus Zehner
Atmos. Chem. Phys., 16, 5705–5720, https://doi.org/10.5194/acp-16-5705-2016, https://doi.org/10.5194/acp-16-5705-2016, 2016
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The ESA-funded SACS-2 and SMASH projects developed and improved dedicated satellite-derived ash plume and sulfur dioxide level assessments. These estimates were validated using ground-based and aircraft lidar measurements. The validation results are promising for most satellite products and are within the estimated uncertainties of each of the comparative data sets. The IASI data show a better consistency concerning the ash optical depth and ash layer height.
Chris Reed, Mathew J. Evans, Piero Di Carlo, James D. Lee, and Lucy J. Carpenter
Atmos. Chem. Phys., 16, 4707–4724, https://doi.org/10.5194/acp-16-4707-2016, https://doi.org/10.5194/acp-16-4707-2016, 2016
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The self-cleaning capacity of the atmosphere in places like Antarctica can be measured by quantifying very low amounts of combustion products that exist in a well-known ratio. When this ratio deviates from 1 it points to the existence of unknown compounds. Several unknown compounds have been theorized to exist but never measured. We have found the method for measuring the ratio of combustion products suffers a bias in remote places, which when taken into account disproves any unknown compounds.
Frank A. F. Winiberg, Terry J. Dillon, Stephanie C. Orr, Christoph B. M Groß, Iustinian Bejan, Charlotte A. Brumby, Matthew J. Evans, Shona C. Smith, Dwayne E. Heard, and Paul W. Seakins
Atmos. Chem. Phys., 16, 4023–4042, https://doi.org/10.5194/acp-16-4023-2016, https://doi.org/10.5194/acp-16-4023-2016, 2016
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OH radicals are important intermediates in the atmosphere, and the high concentrations observed in tropical regions are yet to be fully explained. Radical-radical reactions such as the title reaction can contribute to OH formation. This is the most fully comprehensive study of the CH3C(O)O2 + HO2 reaction with direct observation of products in all reaction channels. The implications of the new measurements on OH, PAN and NOx concentrations are considered via global models.
Maria Zatko, Lei Geng, Becky Alexander, Eric Sofen, and Katarina Klein
Atmos. Chem. Phys., 16, 2819–2842, https://doi.org/10.5194/acp-16-2819-2016, https://doi.org/10.5194/acp-16-2819-2016, 2016
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We have incorporated an idealized snowpack with a nitrate photolysis parameterization into a global chemical transport model (GEOS-Chem) to examine the implications of snow nitrate photolysis for boundary layer chemistry, the recycling and redistribution of reactive nitrogen, and the preservation of ice-core nitrate in ice cores across Antarctica and Greenland. We also examine the sensitivity of these processes to meteorological parameters and chemical, optical, and physical snow properties.
Sophie Bauduin, Lieven Clarisse, Juliette Hadji-Lazaro, Nicolas Theys, Cathy Clerbaux, and Pierre-François Coheur
Atmos. Meas. Tech., 9, 721–740, https://doi.org/10.5194/amt-9-721-2016, https://doi.org/10.5194/amt-9-721-2016, 2016
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The paper presents the development of a new retrieval scheme to infer near-surface sulfur dioxide (SO2) concentrations at a global scale from the Infrared Atmospheric Sounding Interferometer (IASI). It demonstrates the capability of such an instrument to globally monitor anthropogenic SO2 pollution in the case of favourable geophysical conditions, especially high thermal contrast and low humidity.
A.-M. Blechschmidt, A. Richter, J. P. Burrows, L. Kaleschke, K. Strong, N. Theys, M. Weber, X. Zhao, and A. Zien
Atmos. Chem. Phys., 16, 1773–1788, https://doi.org/10.5194/acp-16-1773-2016, https://doi.org/10.5194/acp-16-1773-2016, 2016
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A comprehensive case study of a comma-shaped bromine monoxide plume in the Arctic, which was transported by a polar cyclone and was observed by the GOME-2 satellite sensor over several days, is presented. By making combined use of different kinds of satellite data and numerical models, we demonstrate the important role of the frontal weather system in favouring the bromine activation cycle and blowing snow production, which may have acted as a bromine source during the bromine explosion event.
E. D. Sofen, D. Bowdalo, M. J. Evans, F. Apadula, P. Bonasoni, M. Cupeiro, R. Ellul, I. E. Galbally, R. Girgzdiene, S. Luppo, M. Mimouni, A. C. Nahas, M. Saliba, and K. Tørseth
Earth Syst. Sci. Data, 8, 41–59, https://doi.org/10.5194/essd-8-41-2016, https://doi.org/10.5194/essd-8-41-2016, 2016
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We have brought together all publicly available surface ozone observations from online databases from 1971–2015, with 2200 sites representing regional background conditions appropriate for the evaluation of chemical transport and chemistry-climate models for projects such as the Chemistry-Climate Model Initiative. Gridded data sets of ozone metrics (mean, percentiles, MDA8, SOMO35, etc.) are available from the British Atmospheric Data Centre.
E. D. Sofen, D. Bowdalo, and M. J. Evans
Atmos. Chem. Phys., 16, 1445–1457, https://doi.org/10.5194/acp-16-1445-2016, https://doi.org/10.5194/acp-16-1445-2016, 2016
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We explore the global representativeness of a global surface ozone data set from a range of perspectives (area, biomes, chemical regimes, model uncertainty, model trends). We conclude that the current network fails to provide sufficient constraints for important regions/regimes, leading to uncertainty for a range of atmospheric composition challenges. We suggest 20 new locations for making surface ozone observations, which would significantly enhance our observational capability.
S. Hassinen, D. Balis, H. Bauer, M. Begoin, A. Delcloo, K. Eleftheratos, S. Gimeno Garcia, J. Granville, M. Grossi, N. Hao, P. Hedelt, F. Hendrick, M. Hess, K.-P. Heue, J. Hovila, H. Jønch-Sørensen, N. Kalakoski, A. Kauppi, S. Kiemle, L. Kins, M. E. Koukouli, J. Kujanpää, J.-C. Lambert, R. Lang, C. Lerot, D. Loyola, M. Pedergnana, G. Pinardi, F. Romahn, M. van Roozendael, R. Lutz, I. De Smedt, P. Stammes, W. Steinbrecht, J. Tamminen, N. Theys, L. G. Tilstra, O. N. E. Tuinder, P. Valks, C. Zerefos, W. Zimmer, and I. Zyrichidou
Atmos. Meas. Tech., 9, 383–407, https://doi.org/10.5194/amt-9-383-2016, https://doi.org/10.5194/amt-9-383-2016, 2016
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The three GOME-2 instruments will provide unique and long data sets for atmospheric research and applications. The complete time period will be 2007–2022, including the period of ozone depletion as well as the beginning of ozone layer recovery. The GOME-2 products (ozone, trace gases, aerosols and UV radiation) are important for ozone chemistry, air quality studies, climate modeling, policy monitoring and hazard warnings. The processing and dissemination is done by EUMETSAT O3M SAF project.
T. Sherwen, M. J. Evans, L. J. Carpenter, S. J. Andrews, R. T. Lidster, B. Dix, T. K. Koenig, R. Sinreich, I. Ortega, R. Volkamer, A. Saiz-Lopez, C. Prados-Roman, A. S. Mahajan, and C. Ordóñez
Atmos. Chem. Phys., 16, 1161–1186, https://doi.org/10.5194/acp-16-1161-2016, https://doi.org/10.5194/acp-16-1161-2016, 2016
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Using a global chemical transport model (GEOS-Chem) with additional iodine emissions, chemistry, and deposition we show that iodine is responsible for ~ 9 % of global ozone loss but has negligible impacts on global OH. Uncertainties are large in the chemistry and emissions and future research is needed in both. Measurements of iodine species (especially HOI) would be useful. We believe iodine chemistry should be considered in future chemistry-climate and in air quality modelling.
S. Walter, A. Kock, T. Steinhoff, B. Fiedler, P. Fietzek, J. Kaiser, M. Krol, M. E. Popa, Q. Chen, T. Tanhua, and T. Röckmann
Biogeosciences, 13, 323–340, https://doi.org/10.5194/bg-13-323-2016, https://doi.org/10.5194/bg-13-323-2016, 2016
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Oceans are a source of H2, an indirect greenhouse gas. Measurements constraining the temporal and spatial patterns of oceanic H2 emissions are sparse and although H2 is assumed to be produced mainly biologically, direct evidence for biogenic marine production was lacking. By analyzing the H2 isotopic composition (δD) we were able to constrain the global H2 budget in more detail, verify biogenic production and point to additional sources. We also showed that current models are reasonably working.
E. D. Sofen, M. J. Evans, and A. C. Lewis
Atmos. Chem. Phys., 15, 13627–13632, https://doi.org/10.5194/acp-15-13627-2015, https://doi.org/10.5194/acp-15-13627-2015, 2015
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As an air pollutant, O3 is monitored photometrically to assess compliance with air quality legislation. A recent study found a 1.8% reduction in its absorption cross section, which would lead to an equivalent increase in observed O3 concentrations. We estimate this would increase the number of sites out of compliance with air quality regulations in the EU and US by 20%. We draw attention to how small changes in gas metrology impacts attainment and compliance with legal air quality standards.
Q. Chen, M. E. Popa, A. M. Batenburg, and T. Röckmann
Atmos. Chem. Phys., 15, 13003–13021, https://doi.org/10.5194/acp-15-13003-2015, https://doi.org/10.5194/acp-15-13003-2015, 2015
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We investigated soil production and uptake of H2 and associated isotope effects. Uptake and emission of H2 occurred simultaneously at all sampling sites, with strongest emission where N2 fixing legume was present. The fractionation constant during soil uptake was about 0.945 and it did not show positive correlation with deposition velocity. The isotopic composition of H2 emitted from soil with legume was about -530‰, which is less deuterium-depleted than isotope equilibrium between H2O and H2.
I. De Smedt, T. Stavrakou, F. Hendrick, T. Danckaert, T. Vlemmix, G. Pinardi, N. Theys, C. Lerot, C. Gielen, C. Vigouroux, C. Hermans, C. Fayt, P. Veefkind, J.-F. Müller, and M. Van Roozendael
Atmos. Chem. Phys., 15, 12519–12545, https://doi.org/10.5194/acp-15-12519-2015, https://doi.org/10.5194/acp-15-12519-2015, 2015
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We present the new version of the BIRA-IASB algorithm for the retrieval of H2CO columns from OMI and GOME-2A and B measurements. Validation results at seven stations in Europe, China and Africa confirm the capacity of the satellite measurements to resolve diurnal variations in H2CO columns. Furthermore, vertical profiles derived from MAX-DOAS measurements in Beijing and in Bujumbura are used for a more detailed validation exercise. Finally trends are estimated using 10 years of OMI observations.
R. E. Dunmore, J. R. Hopkins, R. T. Lidster, J. D. Lee, M. J. Evans, A. R. Rickard, A. C. Lewis, and J. F. Hamilton
Atmos. Chem. Phys., 15, 9983–9996, https://doi.org/10.5194/acp-15-9983-2015, https://doi.org/10.5194/acp-15-9983-2015, 2015
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Technological shifts between fuel sources have had unexpected impacts on atmospheric composition and these significant changes can go undetected if source-specific monitoring infrastructure is not in place. We present chemically comprehensive, continuous measurements of organic compounds in a developed megacity (London), that show diesel-related hydrocarbons can dominate reactive carbon and ozone formation potential, highlighting a serious underestimation of this source in emission inventories.
H. M. Walker, D. Stone, T. Ingham, S. Vaughan, M. Cain, R. L. Jones, O. J. Kennedy, M. McLeod, B. Ouyang, J. Pyle, S. Bauguitte, B. Bandy, G. Forster, M. J. Evans, J. F. Hamilton, J. R. Hopkins, J. D. Lee, A. C. Lewis, R. T. Lidster, S. Punjabi, W. T. Morgan, and D. E. Heard
Atmos. Chem. Phys., 15, 8179–8200, https://doi.org/10.5194/acp-15-8179-2015, https://doi.org/10.5194/acp-15-8179-2015, 2015
P. Achakulwisut, L. J. Mickley, L. T. Murray, A. P. K. Tai, J. O. Kaplan, and B. Alexander
Atmos. Chem. Phys., 15, 7977–7998, https://doi.org/10.5194/acp-15-7977-2015, https://doi.org/10.5194/acp-15-7977-2015, 2015
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The atmosphere’s oxidative capacity determines the lifetime of many trace gases important to climate, chemistry, and human health. Yet uncertainties remain about its past variations, its controlling factors, and the radiative forcing of short-lived species it influences. To reduce these uncertainties, we must better quantify the natural emissions and chemical reaction mechanisms of organic compounds in the atmosphere, which play a role in governing the oxidative capacity.
L. K. Whalley, D. Stone, I. J. George, S. Mertes, D. van Pinxteren, A. Tilgner, H. Herrmann, M. J. Evans, and D. E. Heard
Atmos. Chem. Phys., 15, 3289–3301, https://doi.org/10.5194/acp-15-3289-2015, https://doi.org/10.5194/acp-15-3289-2015, 2015
L. Geng, J. Cole-Dai, B. Alexander, J. Erbland, J. Savarino, A. J. Schauer, E. J. Steig, P. Lin, Q. Fu, and M. C. Zatko
Atmos. Chem. Phys., 14, 13361–13376, https://doi.org/10.5194/acp-14-13361-2014, https://doi.org/10.5194/acp-14-13361-2014, 2014
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Examinations on snowpit and firn core results from Summit, Greenland suggest that there are two mechanisms leading to the observed double nitrate peaks in some years in the industrial era: 1) long-rang transport of nitrate and 2) enhanced local photochemical production of nitrate. Both of these mechanisms are related to pollution transport, as the additional nitrate from either direct transport or enhanced local photochemistry requires enhanced nitrogen sources from anthropogenic emissions.
T. Wang, F. Hendrick, P. Wang, G. Tang, K. Clémer, H. Yu, C. Fayt, C. Hermans, C. Gielen, J.-F. Müller, G. Pinardi, N. Theys, H. Brenot, and M. Van Roozendael
Atmos. Chem. Phys., 14, 11149–11164, https://doi.org/10.5194/acp-14-11149-2014, https://doi.org/10.5194/acp-14-11149-2014, 2014
S. Choi, J. Joiner, Y. Choi, B. N. Duncan, A. Vasilkov, N. Krotkov, and E. Bucsela
Atmos. Chem. Phys., 14, 10565–10588, https://doi.org/10.5194/acp-14-10565-2014, https://doi.org/10.5194/acp-14-10565-2014, 2014
E. D. Sofen, B. Alexander, E. J. Steig, M. H. Thiemens, S. A. Kunasek, H. M. Amos, A. J. Schauer, M. G. Hastings, J. Bautista, T. L. Jackson, L. E. Vogel, J. R. McConnell, D. R. Pasteris, and E. S. Saltzman
Atmos. Chem. Phys., 14, 5749–5769, https://doi.org/10.5194/acp-14-5749-2014, https://doi.org/10.5194/acp-14-5749-2014, 2014
H. Brenot, N. Theys, L. Clarisse, J. van Geffen, J. van Gent, M. Van Roozendael, R. van der A, D. Hurtmans, P.-F. Coheur, C. Clerbaux, P. Valks, P. Hedelt, F. Prata, O. Rasson, K. Sievers, and C. Zehner
Nat. Hazards Earth Syst. Sci., 14, 1099–1123, https://doi.org/10.5194/nhess-14-1099-2014, https://doi.org/10.5194/nhess-14-1099-2014, 2014
L. T. Murray, L. J. Mickley, J. O. Kaplan, E. D. Sofen, M. Pfeiffer, and B. Alexander
Atmos. Chem. Phys., 14, 3589–3622, https://doi.org/10.5194/acp-14-3589-2014, https://doi.org/10.5194/acp-14-3589-2014, 2014
L. Clarisse, P.-F. Coheur, N. Theys, D. Hurtmans, and C. Clerbaux
Atmos. Chem. Phys., 14, 3095–3111, https://doi.org/10.5194/acp-14-3095-2014, https://doi.org/10.5194/acp-14-3095-2014, 2014
D. Stone, M. J. Evans, H. Walker, T. Ingham, S. Vaughan, B. Ouyang, O. J. Kennedy, M. W. McLeod, R. L. Jones, J. Hopkins, S. Punjabi, R. Lidster, J. F. Hamilton, J. D. Lee, A. C. Lewis, L. J. Carpenter, G. Forster, D. E. Oram, C. E. Reeves, S. Bauguitte, W. Morgan, H. Coe, E. Aruffo, C. Dari-Salisburgo, F. Giammaria, P. Di Carlo, and D. E. Heard
Atmos. Chem. Phys., 14, 1299–1321, https://doi.org/10.5194/acp-14-1299-2014, https://doi.org/10.5194/acp-14-1299-2014, 2014
P. M. Edwards, M. J. Evans, K. L. Furneaux, J. Hopkins, T. Ingham, C. Jones, J. D. Lee, A. C. Lewis, S. J. Moller, D. Stone, L. K. Whalley, and D. E. Heard
Atmos. Chem. Phys., 13, 9497–9514, https://doi.org/10.5194/acp-13-9497-2013, https://doi.org/10.5194/acp-13-9497-2013, 2013
N. Theys, R. Campion, L. Clarisse, H. Brenot, J. van Gent, B. Dils, S. Corradini, L. Merucci, P.-F. Coheur, M. Van Roozendael, D. Hurtmans, C. Clerbaux, S. Tait, and F. Ferrucci
Atmos. Chem. Phys., 13, 5945–5968, https://doi.org/10.5194/acp-13-5945-2013, https://doi.org/10.5194/acp-13-5945-2013, 2013
J. R. Pierce, M. J. Evans, C. E. Scott, S. D. D'Andrea, D. K. Farmer, E. Swietlicki, and D. V. Spracklen
Atmos. Chem. Phys., 13, 3163–3176, https://doi.org/10.5194/acp-13-3163-2013, https://doi.org/10.5194/acp-13-3163-2013, 2013
A. E. Jones, E. W. Wolff, N. Brough, S. J.-B. Bauguitte, R. Weller, M. Yela, M. Navarro-Comas, H. A. Ochoa, and N. Theys
Atmos. Chem. Phys., 13, 1457–1467, https://doi.org/10.5194/acp-13-1457-2013, https://doi.org/10.5194/acp-13-1457-2013, 2013
A. C. Lewis, M. J. Evans, J. R. Hopkins, S. Punjabi, K. A. Read, R. M. Purvis, S. J. Andrews, S. J. Moller, L. J. Carpenter, J. D. Lee, A. R. Rickard, P. I. Palmer, and M. Parrington
Atmos. Chem. Phys., 13, 851–867, https://doi.org/10.5194/acp-13-851-2013, https://doi.org/10.5194/acp-13-851-2013, 2013
Related subject area
Subject: Aerosols | Research Activity: Atmospheric Modelling and Data Analysis | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
Modeling the drivers of fine PM pollution over Central Europe: impacts and contributions of emissions from different sources
Reaction of SO3 with H2SO4 and its implications for aerosol particle formation in the gas phase and at the air–water interface
Weakened aerosol–radiation interaction exacerbating ozone pollution in eastern China since China's clean air actions
Uncertainties from biomass burning aerosols in air quality models obscure public health impacts in Southeast Asia
Oxidative potential apportionment of atmospheric PM1: a new approach combining high-sensitive online analysers for chemical composition and offline OP measurement technique
Aqueous-phase chemistry of glyoxal with multifunctional reduced nitrogen compounds: a potential missing route for secondary brown carbon
An updated modeling framework to simulate Los Angeles air quality – Part 1: Model development, evaluation, and source apportionment
Frequent haze events associated with transport and stagnation over the corridor between the North China Plain and Yangtze River Delta
Evaluation of WRF-Chem-simulated meteorology and aerosols over northern India during the severe pollution episode of 2016
How well are aerosol–cloud interactions represented in climate models? – Part 1: Understanding the sulfate aerosol production from the 2014–15 Holuhraun eruption
pH regulates the formation of organosulfates and inorganic sulfate from organic peroxide reaction with dissolved SO2 in aquatic media
Technical note: Accurate, reliable, and high-resolution air quality predictions by improving the Copernicus Atmosphere Monitoring Service using a novel statistical post-processing method
Contribution of intermediate-volatility organic compounds from on-road transport to secondary organic aerosol levels in Europe
Secondary Organic Aerosols Derived from Intermediate Volatility n-Alkanes Adopt Low Viscous Phase State
Development of an integrated model framework for multi-air-pollutant exposure assessments in high-density cities
Observation-Constrained Kinetic Modelling of Isoprene SOA Formation in the Atmosphere
CAMx–UNIPAR simulation of secondary organic aerosol mass formed from multiphase reactions of hydrocarbons under the Central Valley urban atmospheres of California
Impact of urbanization on fine particulate matter concentrations over central Europe
Measurement report: Assessing the impacts of emission uncertainty on aerosol optical properties and radiative forcing from biomass burning in peninsular Southeast Asia
Global source apportionment of aerosols into major emission regions and sectors over 1850–2017
Significant impact of urban-tree biogenic emissions on air quality estimated by a bottom-up inventory and chemistry-transport modeling
The Emissions Model Intercomparison Project (Emissions-MIP): quantifying model sensitivity to emission characteristics
Dynamics-based estimates of decline trend with fine temporal variations in China's PM2.5 emissions
Modeling atmospheric brown carbon in the GISS ModelE Earth system model
Dual roles of inorganic aqueous phase on SOA growth from benzene and phenol
Effects of simulated secondary organic aerosol water on PM1 levels and composition over the US
Reactive organic carbon air emissions from mobile sources in the United States
Development and evaluation of processes affecting simulation of diel fine particulate matter variation in the GEOS-Chem model
Substantially positive contributions of new particle formation to cloud condensation nuclei under low supersaturation in China based on numerical model improvements
Evolution of atmospheric age of particles and its implications for the formation of a severe haze event in eastern China
A multimodel evaluation of the potential impact of shipping on particle species in the Mediterranean Sea
Investigating the contribution of grown new particles to cloud condensation nuclei with largely varying pre-existing particles – Part 2: Modeling chemical drivers and 3-D NPF occurrence
How does tropospheric VOC chemistry affect climate? An investigation of preindustrial control simulations using the Community Earth System Model version 2
Anthropogenic amplification of biogenic secondary organic aerosol production
A dynamic parameterization of sulfuric acid–dimethylamine nucleation and its application in three-dimensional modeling
Modeling dust mineralogical composition: sensitivity to soil mineralogy atlases and their expected climate impacts
Assessment of the impacts of cloud chemistry on surface SO2 and sulfate levels in typical regions of China
Impact of Landes forest fires on air quality in France during the 2022 summer
Global nitrogen and sulfur deposition mapping using a measurement–model fusion approach
Comprehensive simulations of new particle formation events in Beijing with a cluster dynamics–multicomponent sectional model
Implications of differences between recent anthropogenic aerosol emission inventories for diagnosed AOD and radiative forcing from 1990 to 2019
Unbalanced emission reductions of different species and sectors in China during COVID-19 lockdown derived by multi-species surface observation assimilation
Simulating organic aerosol in Delhi with WRF-Chem using the volatility-basis-set approach: exploring model uncertainty with a Gaussian process emulator
Modelling wintertime sea-spray aerosols under Arctic haze conditions
Impact of solar geoengineering on wildfires in the 21st century in CESM2/WACCM6
Linking gas, particulate, and toxic endpoints to air emissions in the Community Regional Atmospheric Chemistry Multiphase Mechanism (CRACMM)
Contribution of regional aerosol nucleation to low-level CCN in an Amazonian deep convective environment: results from a regionally nested global model
Coarse particulate matter air quality in East Asia: implications for fine particulate nitrate
Foreign emissions exacerbate PM2.5 pollution in China through nitrate chemistry
Analysis of new particle formation events and comparisons to simulations of particle number concentrations based on GEOS-Chem–advanced particle microphysics in Beijing, China
Lukáš Bartík, Peter Huszár, Jan Karlický, Ondřej Vlček, and Kryštof Eben
Atmos. Chem. Phys., 24, 4347–4387, https://doi.org/10.5194/acp-24-4347-2024, https://doi.org/10.5194/acp-24-4347-2024, 2024
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The presented study deals with the attribution of fine particulate matter (PM2.5) concentrations to anthropogenic emissions over Central Europe using regional-scale models. It calculates the present-day contributions of different emissions sectors to concentrations of PM2.5 and its secondary components. Moreover, the study investigates the effect of chemical nonlinearities by using multiple source attribution methods and secondary organic aerosol calculation methods.
Rui Wang, Yang Cheng, Shasha Chen, Rongrong Li, Yue Hu, Xiaokai Guo, Tianlei Zhang, Fengmin Song, and Hao Li
Atmos. Chem. Phys., 24, 4029–4046, https://doi.org/10.5194/acp-24-4029-2024, https://doi.org/10.5194/acp-24-4029-2024, 2024
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We used quantum chemical calculations, Born–Oppenheimer molecular dynamics simulations, and the ACDC kinetic model to characterize SO3–H2SO4 interaction in the gas phase and at the air–water interface and to study the effect of H2S2O7 on H2SO4–NH3-based clusters. The work expands our understanding of new pathways for the loss of SO3 in acidic polluted areas and helps reveal some missing sources of NPF in metropolitan industrial regions and understand the atmospheric organic–sulfur cycle better.
Hao Yang, Lei Chen, Hong Liao, Jia Zhu, Wenjie Wang, and Xin Li
Atmos. Chem. Phys., 24, 4001–4015, https://doi.org/10.5194/acp-24-4001-2024, https://doi.org/10.5194/acp-24-4001-2024, 2024
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The present study quantifies the response of aerosol–radiation interaction (ARI) to anthropogenic emission reduction from 2013 to 2017, with the main focus on the contribution to changed O3 concentrations over eastern China both in summer and winter using the WRF-Chem model. The weakened ARI due to decreased anthropogenic emission aggravates the summer (winter) O3 pollution by +0.81 ppb (+0.63 ppb), averaged over eastern China.
Margaret R. Marvin, Paul I. Palmer, Fei Yao, Mohd Talib Latif, and Md Firoz Khan
Atmos. Chem. Phys., 24, 3699–3715, https://doi.org/10.5194/acp-24-3699-2024, https://doi.org/10.5194/acp-24-3699-2024, 2024
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We use an atmospheric chemistry model to investigate aerosols emitted from fire activity across Southeast Asia. We find that the limited nature of measurements in this region leads to large uncertainties that significantly hinder the model representation of these aerosols and their impacts on air quality. As a result, the number of monthly attributable deaths is underestimated by as many as 4500, particularly in March at the peak of the mainland burning season.
Julie Camman, Benjamin Chazeau, Nicolas Marchand, Amandine Durand, Grégory Gille, Ludovic Lanzi, Jean-Luc Jaffrezo, Henri Wortham, and Gaëlle Uzu
Atmos. Chem. Phys., 24, 3257–3278, https://doi.org/10.5194/acp-24-3257-2024, https://doi.org/10.5194/acp-24-3257-2024, 2024
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Fine particle (PM1) pollution is a major health issue in the city of Marseille, which is subject to numerous pollution sources. Sampling carried out during the summer enabled a fine characterization of the PM1 sources and their oxidative potential, a promising new metric as a proxy for health impact. PM1 came mainly from combustion sources, secondary ammonium sulfate, and organic nitrate, while the oxidative potential of PM1 came from these sources and from resuspended dust in the atmosphere.
Yuemeng Ji, Zhang Shi, Wenjian Li, Jiaxin Wang, Qiuju Shi, Yixin Li, Lei Gao, Ruize Ma, Weijun Lu, Lulu Xu, Yanpeng Gao, Guiying Li, and Taicheng An
Atmos. Chem. Phys., 24, 3079–3091, https://doi.org/10.5194/acp-24-3079-2024, https://doi.org/10.5194/acp-24-3079-2024, 2024
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The formation mechanisms for secondary brown carbon (SBrC) contributed by multifunctional reduced nitrogen compounds (RNCs) remain unclear. Hence, from combined laboratory experiments and quantum chemical calculations, we investigated the heterogeneous reactions of glyoxal (GL) with multifunctional RNCs, which are driven by four-step indirect nucleophilic addition reactions. Our results show a possible missing source for SBrC formation on urban, regional, and global scales.
Elyse A. Pennington, Yuan Wang, Benjamin C. Schulze, Karl M. Seltzer, Jiani Yang, Bin Zhao, Zhe Jiang, Hongru Shi, Melissa Venecek, Daniel Chau, Benjamin N. Murphy, Christopher M. Kenseth, Ryan X. Ward, Havala O. T. Pye, and John H. Seinfeld
Atmos. Chem. Phys., 24, 2345–2363, https://doi.org/10.5194/acp-24-2345-2024, https://doi.org/10.5194/acp-24-2345-2024, 2024
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To assess the air quality in Los Angeles (LA), we improved the CMAQ model by using dynamic traffic emissions and new secondary organic aerosol schemes to represent volatile chemical products. Source apportionment demonstrates that the urban areas of the LA Basin and vicinity are NOx-saturated, with the largest sensitivity of O3 to changes in volatile organic compounds in the urban core. The improvement and remaining issues shed light on the future direction of the model development.
Feifan Yan, Hang Su, Yafang Cheng, Rujin Huang, Hong Liao, Ting Yang, Yuanyuan Zhu, Shaoqing Zhang, Lifang Sheng, Wenbin Kou, Xinran Zeng, Shengnan Xiang, Xiaohong Yao, Huiwang Gao, and Yang Gao
Atmos. Chem. Phys., 24, 2365–2376, https://doi.org/10.5194/acp-24-2365-2024, https://doi.org/10.5194/acp-24-2365-2024, 2024
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PM2.5 pollution is a major air quality issue deteriorating human health, and previous studies mostly focus on regions like the North China Plain and Yangtze River Delta. However, the characteristics of PM2.5 concentrations between these two regions are studied less often. Focusing on the transport corridor region, we identify an interesting seesaw transport phenomenon with stagnant weather conditions, conducive to PM2.5 accumulation over this region, resulting in large health effects.
Prerita Agarwal, David S. Stevenson, and Mathew R. Heal
Atmos. Chem. Phys., 24, 2239–2266, https://doi.org/10.5194/acp-24-2239-2024, https://doi.org/10.5194/acp-24-2239-2024, 2024
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Air pollution levels across northern India are amongst some of the worst in the world, with episodic and hazardous haze events. Here, the ability of the WRF-Chem model to predict air quality over northern India is assessed against several datasets. Whilst surface wind speed and particle pollution peaks are over- and underestimated, respectively, meteorology and aerosol trends are adequately captured, and we conclude it is suitable for investigating severe particle pollution events.
George Jordan, Florent Malavelle, Ying Chen, Amy Peace, Eliza Duncan, Daniel G. Partridge, Paul Kim, Duncan Watson-Parris, Toshihiko Takemura, David Neubauer, Gunnar Myhre, Ragnhild Skeie, Anton Laakso, and James Haywood
Atmos. Chem. Phys., 24, 1939–1960, https://doi.org/10.5194/acp-24-1939-2024, https://doi.org/10.5194/acp-24-1939-2024, 2024
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The 2014–15 Holuhraun eruption caused a huge aerosol plume in an otherwise unpolluted region, providing a chance to study how aerosol alters cloud properties. This two-part study uses observations and models to quantify this relationship’s impact on the Earth’s energy budget. Part 1 suggests the models capture the observed spatial and chemical evolution of the plume, yet no model plume is exact. Understanding these differences is key for Part 2, where changes to cloud properties are explored.
Lin Du, Xiaofan Lv, Makroni Lily, Kun Li, and Narcisse Tsona Tchinda
Atmos. Chem. Phys., 24, 1841–1853, https://doi.org/10.5194/acp-24-1841-2024, https://doi.org/10.5194/acp-24-1841-2024, 2024
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This study explores the pH effect on the reaction of dissolved SO2 with selected organic peroxides. Results show that the formation of organic and/or inorganic sulfate from these peroxides strongly depends on their electronic structures, and these processes are likely to alter the chemical composition of dissolved organic matter in different ways. The rate constants of these reactions exhibit positive pH and temperature dependencies within pH 1–10 and 240–340 K ranges.
Angelo Riccio and Elena Chianese
Atmos. Chem. Phys., 24, 1673–1689, https://doi.org/10.5194/acp-24-1673-2024, https://doi.org/10.5194/acp-24-1673-2024, 2024
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Starting from the Copernicus Atmosphere Monitoring Service (CAMS), we provided a novel ensemble statistical post-processing approach to improve their air quality predictions. Our approach is able to provide reliable short-term forecasts of pollutant concentrations, which is a key challenge in supporting national authorities in their tasks related to EU Air Quality Directives, such as planning and reporting the state of air quality to the citizens.
Stella E. I. Manavi and Spyros N. Pandis
Atmos. Chem. Phys., 24, 891–909, https://doi.org/10.5194/acp-24-891-2024, https://doi.org/10.5194/acp-24-891-2024, 2024
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Organic vapors of intermediate volatility have often been neglected as sources of atmospheric organic aerosol. In this work we use a new approach for their simulation and quantify the contribution of these compounds emitted by transportation sources (gasoline and diesel vehicles) to particulate matter over Europe. The estimated secondary organic aerosol levels are on average 60 % higher than predicted by previous approaches. However, these estimates are probably lower limits.
Tommaso Galeazzo, Bernard Aumont, Marie Camredon, Richard Valorso, Yong B. Lim, Paul J. Ziemann, and Manabu Shiraiwa
EGUsphere, https://doi.org/10.5194/egusphere-2024-51, https://doi.org/10.5194/egusphere-2024-51, 2024
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SOA derived from n-alkanes is a major component of anthropogenic particulate matter. We provide a comprehensive analysis of n-alkane SOA by explicit chemistry modeling, machine learning, and laboratory experiments, showing that n-alkane SOA adopt low viscous semisolid or liquid states. Our results indicate little kinetic limitations of mass accommodation in SOA formation, supporting the application of equilibrium partitioning for simulating n-alkane SOA in large-scale atmospheric models.
Zhiyuan Li, Kin-Fai Ho, Harry Fung Lee, and Steve Hung Lam Yim
Atmos. Chem. Phys., 24, 649–661, https://doi.org/10.5194/acp-24-649-2024, https://doi.org/10.5194/acp-24-649-2024, 2024
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This study developed an integrated model framework for accurate multi-air-pollutant exposure assessments in high-density and high-rise cities. Following the proposed integrated model framework, we established multi-air-pollutant exposure models for four major PM10 chemical species as well as four criteria air pollutants with R2 values ranging from 0.73 to 0.93. The proposed framework serves as an important tool for combined exposure assessment in epidemiological studies.
Chuanyang Shen, Xiaoyan Yang, Joel Thornton, John Shilling, Chenyang Bi, Gabriel Isaacman-VanWertz, and Haofei Zhang
EGUsphere, https://doi.org/10.5194/egusphere-2024-97, https://doi.org/10.5194/egusphere-2024-97, 2024
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In this work, a multiphase condensed isoprene oxidation mechanism was developed to simulate isoprene SOA formation from chamber and field studies. Our results show that the measured isoprene SOA mass can be reasonably reproduced using the new mechanism. The simulation results indicate that multifunctional low-volatility products contribute significantly to total isoprene SOA. Our findings emphasize that the pathways to produce these low-volatility species should be considered in models.
Yujin Jo, Myoseon Jang, Sanghee Han, Azad Madhu, Bonyoung Koo, Yiqin Jia, Zechen Yu, Soontae Kim, and Jinsoo Park
Atmos. Chem. Phys., 24, 487–508, https://doi.org/10.5194/acp-24-487-2024, https://doi.org/10.5194/acp-24-487-2024, 2024
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The CAMx–UNIPAR model simulated the SOA budget formed via multiphase reactions of hydrocarbons and the impact of emissions and climate on SOA characteristics under California’s urban environments during winter 2018. SOA growth was dominated by daytime oxidation of long-chain alkanes and nighttime terpene oxidation with O3 and NO−3 radicals. The spatial distributions of anthropogenic SOA were affected by the northwesterly wind, whereas those of biogenic SOA were insensitive to wind directions.
Peter Huszar, Alvaro Patricio Prieto Perez, Lukáš Bartík, Jan Karlický, and Anahi Villalba-Pradas
Atmos. Chem. Phys., 24, 397–425, https://doi.org/10.5194/acp-24-397-2024, https://doi.org/10.5194/acp-24-397-2024, 2024
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Urbanization transforms rural land into artificial land, while due to human activities, it also introduces a great quantity of emissions. We quantify the impact of urbanization on the final particulate matter pollutant levels by looking not only at these emissions, but also at the way urban land cover influences meteorological conditions, how the removal of pollutants changes due to urban land cover, and how biogenic emissions from vegetation change due to less vegetation in urban areas.
Yinbao Jin, Yiming Liu, Xiao Lu, Xiaoyang Chen, Ao Shen, Haofan Wang, Yinping Cui, Yifei Xu, Siting Li, Jian Liu, Ming Zhang, Yingying Ma, and Qi Fan
Atmos. Chem. Phys., 24, 367–395, https://doi.org/10.5194/acp-24-367-2024, https://doi.org/10.5194/acp-24-367-2024, 2024
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This study aims to address these issues by evaluating eight independent biomass burning (BB) emission inventories (GFED, FINN1.5, FINN2.5 MOS, FINN2.5 MOSVIS, GFAS, FEER, QFED, and IS4FIRES) using the WRF-Chem model and analyzing their impact on aerosol optical properties (AOPs) and direct radiative forcing (DRF) during wildfire events in peninsular Southeast Asia (PSEA) that occurred in March 2019.
Yang Yang, Shaoxuan Mou, Hailong Wang, Pinya Wang, Baojie Li, and Hong Liao
EGUsphere, https://doi.org/10.5194/egusphere-2023-2552, https://doi.org/10.5194/egusphere-2023-2552, 2024
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We quantify the variations in anthropogenic aerosol concentrations, source contributions, and their subsequent radiative impact in four major emission regions during four historical period. Due to industrial development and the implementation of different economic policies, sources of anthropogenic aerosols show different variations, which has important implications for the pollution prevention/control measures and decision making for global collaboration.
Alice Maison, Lya Lugon, Soo-Jin Park, Alexia Baudic, Christopher Cantrell, Florian Couvidat, Barbara D'Anna, Claudia Di Biagio, Aline Gratien, Valérie Gros, Carmen Kalalian, Julien Kammer, Vincent Michoud, Jean-Eudes Petit, Marwa Shahin, Leila Simon, Myrto Valari, Jérémy Vigneron, Andrée Tuzet, and Karine Sartelet
EGUsphere, https://doi.org/10.5194/egusphere-2023-2786, https://doi.org/10.5194/egusphere-2023-2786, 2023
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This study presents the development of a bottom-up inventory of urban-tree biogenic emissions. Emissions are computed for each tree based on their location and characteristics and are integrated in the regional air-quality model WRF-CHIMERE. The impact of these biogenic emissions on air quality is quantified for June–July 2022. Over Paris city, urban trees increase the concentrations of particulate organic matter by 4.6 %, of PM2.5 by 0.6 % and of ozone by 1.0 % on average over the two months.
Hamza Ahsan, Hailong Wang, Jingbo Wu, Mingxuan Wu, Steven J. Smith, Susanne Bauer, Harrison Suchyta, Dirk Olivié, Gunnar Myhre, Hitoshi Matsui, Huisheng Bian, Jean-François Lamarque, Ken Carslaw, Larry Horowitz, Leighton Regayre, Mian Chin, Michael Schulz, Ragnhild Bieltvedt Skeie, Toshihiko Takemura, and Vaishali Naik
Atmos. Chem. Phys., 23, 14779–14799, https://doi.org/10.5194/acp-23-14779-2023, https://doi.org/10.5194/acp-23-14779-2023, 2023
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We examine the impact of the assumed effective height of SO2 injection, SO2 and BC emission seasonality, and the assumed fraction of SO2 emissions injected as SO4 on climate and chemistry model results. We find that the SO2 injection height has a large impact on surface SO2 concentrations and, in some models, radiative flux. These assumptions are a
hiddensource of inter-model variability and may be leading to bias in some climate model results.
Zhen Peng, Lili Lei, Zhe-Min Tan, Meigen Zhang, Aijun Ding, and Xingxia Kou
Atmos. Chem. Phys., 23, 14505–14520, https://doi.org/10.5194/acp-23-14505-2023, https://doi.org/10.5194/acp-23-14505-2023, 2023
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Annual PM2.5 emissions in China consistently decreased by about 3% to 5% from 2017 to 2020 with spatial variations and seasonal dependencies. High-temporal-resolution and dynamics-based PM2.5 emission estimates provide quantitative diurnal variations for each season. Significant reductions in PM2.5 emissions in the North China Plain and northeast of China in 2020 were caused by COVID-19.
Maegan A. DeLessio, Kostas Tsigaridis, Susanne E. Bauer, Jacek Chowdhary, and Gregory L. Schuster
EGUsphere, https://doi.org/10.5194/egusphere-2023-2472, https://doi.org/10.5194/egusphere-2023-2472, 2023
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This study presents the first explicit representation of brown carbon aerosols in the GISS ModelE Earth system model (ESM). Model sensitivity to a range of brown carbon parameters, as well as model performance compared to AERONET and MODIS retrievals of total aerosol properties, was assessed. General recommendations for incorporating brown carbon into ESMs are also included.
Jiwon Choi, Myoseon Jang, and Spencer Blau
EGUsphere, https://doi.org/10.5194/egusphere-2023-2461, https://doi.org/10.5194/egusphere-2023-2461, 2023
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A persistent phenoxy radical (PPR) effectively forms via a heterogeneous reaction of phenol and phenol-related products in the presence of wet-inorganic aerosol. These PPR can catalytically consume ozone during a NOx cycle and negatively influence SOA formation. SOA formation from phenol or benzene is simulated using the UNIPAR model which predicted SOA formation via multiphase reactions of hydrocarbons and compared with chamber data obtained under varying NOx levels, humidity, and seed types.
Stylianos Kakavas, Spyros N. Pandis, and Athanasios Nenes
Atmos. Chem. Phys., 23, 13555–13564, https://doi.org/10.5194/acp-23-13555-2023, https://doi.org/10.5194/acp-23-13555-2023, 2023
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Water uptake from organic species in aerosol can affect the partitioning of semi-volatile inorganic compounds but are not considered in global and chemical transport models. We address this with a version of the PM-CAMx model that considers such organic water effects and use it to carry out 1-year aerosol simulations over the continental US. We show that such organic water impacts can increase dry PM1 levels by up to 2 μg m-3 when RH levels and PM1 concentrations are high.
Benjamin N. Murphy, Darrell Sonntag, Karl M. Seltzer, Havala O. T. Pye, Christine Allen, Evan Murray, Claudia Toro, Drew R. Gentner, Cheng Huang, Shantanu Jathar, Li Li, Andrew A. May, and Allen L. Robinson
Atmos. Chem. Phys., 23, 13469–13483, https://doi.org/10.5194/acp-23-13469-2023, https://doi.org/10.5194/acp-23-13469-2023, 2023
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We update methods for calculating organic particle and vapor emissions from mobile sources in the USA. Conventionally, particulate matter (PM) and volatile organic carbon (VOC) are speciated without consideration of primary semivolatile emissions. Our methods integrate state-of-the-science speciation profiles and correct for common artifacts when sampling emissions in a laboratory. We quantify impacts of the emission updates on ambient pollution with the Community Multiscale Air Quality model.
Yanshun Li, Randall V. Martin, Chi Li, Brian L. Boys, Aaron van Donkelaar, Jun Meng, and Jeffrey R. Pierce
Atmos. Chem. Phys., 23, 12525–12543, https://doi.org/10.5194/acp-23-12525-2023, https://doi.org/10.5194/acp-23-12525-2023, 2023
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We developed and evaluated processes affecting within-day (diel) variability in PM2.5 concentrations in a chemical transport model over the contiguous US. Diel variability in PM2.5 for the contiguous US is driven by early-morning accumulation into a shallow mixed layer, decreases from mid-morning through afternoon with mixed-layer growth, increases from mid-afternoon through evening as the mixed-layer collapses, and decreases overnight as emissions decrease.
Chupeng Zhang, Shangfei Hai, Yang Gao, Yuhang Wang, Shaoqing Zhang, Lifang Sheng, Bin Zhao, Shuxiao Wang, Jingkun Jiang, Xin Huang, Xiaojing Shen, Junying Sun, Aura Lupascu, Manish Shrivastava, Jerome D. Fast, Wenxuan Cheng, Xiuwen Guo, Ming Chu, Nan Ma, Juan Hong, Qiaoqiao Wang, Xiaohong Yao, and Huiwang Gao
Atmos. Chem. Phys., 23, 10713–10730, https://doi.org/10.5194/acp-23-10713-2023, https://doi.org/10.5194/acp-23-10713-2023, 2023
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New particle formation is an important source of atmospheric particles, exerting critical influences on global climate. Numerical models are vital tools to understanding atmospheric particle evolution, which, however, suffer from large biases in simulating particle numbers. Here we improve the model chemical processes governing particle sizes and compositions. The improved model reveals substantial contributions of newly formed particles to climate through effects on cloud condensation nuclei.
Xiaodong Xie, Jianlin Hu, Momei Qin, Song Guo, Min Hu, Dongsheng Ji, Hongli Wang, Shengrong Lou, Cheng Huang, Chong Liu, Hongliang Zhang, Qi Ying, Hong Liao, and Yuanhang Zhang
Atmos. Chem. Phys., 23, 10563–10578, https://doi.org/10.5194/acp-23-10563-2023, https://doi.org/10.5194/acp-23-10563-2023, 2023
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The atmospheric age of particles reflects how long particles have been formed and suspended in the atmosphere, which is closely associated with the evolution processes of particles. An analysis of the atmospheric age of PM2.5 provides a unique perspective on the evolution processes of different PM2.5 components. The results also shed lights on how to design effective emission control actions under unfavorable meteorological conditions.
Lea Fink, Matthias Karl, Volker Matthias, Sonia Oppo, Richard Kranenburg, Jeroen Kuenen, Sara Jutterström, Jana Moldanova, Elisa Majamäki, and Jukka-Pekka Jalkanen
Atmos. Chem. Phys., 23, 10163–10189, https://doi.org/10.5194/acp-23-10163-2023, https://doi.org/10.5194/acp-23-10163-2023, 2023
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The Mediterranean Sea is a heavily trafficked shipping area, and air quality monitoring stations in numerous cities along the Mediterranean coast have detected high levels of air pollutants originating from shipping emissions. The current study investigates how existing restrictions on shipping-related emissions to the atmosphere ensure compliance with legislation. Focus was laid on fine particles and particle species, which were simulated with five different chemical transport models.
Ming Chu, Xing Wei, Shangfei Hai, Yang Gao, Huiwang Gao, Yujiao Zhu, Biwu Chu, Nan Ma, Juan Hong, Yele Sun, and Xiaohong Yao
EGUsphere, https://doi.org/10.5194/egusphere-2023-540, https://doi.org/10.5194/egusphere-2023-540, 2023
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We used a 20-bin WRF-Chem model to simulate NPF events in the NCP during a three-week observational period in the summer of 2019. The model was able to reproduce the observations during June 29–July 6, which was characterized by a high frequency of NPF occurrence.
Noah A. Stanton and Neil F. Tandon
Atmos. Chem. Phys., 23, 9191–9216, https://doi.org/10.5194/acp-23-9191-2023, https://doi.org/10.5194/acp-23-9191-2023, 2023
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Chemistry in Earth’s atmosphere has a potentially strong but very uncertain impact on climate. Past attempts to fully model chemistry in Earth’s troposphere (the lowest layer of the atmosphere) typically simplified the representation of Earth’s surface, which in turn limited the ability to simulate changes in climate. The cutting-edge model that we use in this study does not require such simplification, and we use it to examine the climate effects of chemical interactions in the troposphere.
Yiqi Zheng, Larry W. Horowitz, Raymond Menzel, David J. Paynter, Vaishali Naik, Jingyi Li, and Jingqiu Mao
Atmos. Chem. Phys., 23, 8993–9007, https://doi.org/10.5194/acp-23-8993-2023, https://doi.org/10.5194/acp-23-8993-2023, 2023
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Biogenic secondary organic aerosols (SOAs) account for a large fraction of fine aerosol at the global scale. Using long-term measurements and a climate model, we investigate anthropogenic impacts on biogenic SOA at both decadal and centennial timescales. Results show that despite reductions in biogenic precursor emissions, SOA has been strongly amplified by anthropogenic emissions since the preindustrial era and exerts a cooling radiative forcing.
Yuyang Li, Jiewen Shen, Bin Zhao, Runlong Cai, Shuxiao Wang, Yang Gao, Manish Shrivastava, Da Gao, Jun Zheng, Markku Kulmala, and Jingkun Jiang
Atmos. Chem. Phys., 23, 8789–8804, https://doi.org/10.5194/acp-23-8789-2023, https://doi.org/10.5194/acp-23-8789-2023, 2023
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We set up a new parameterization for 1.4 nm particle formation rates from sulfuric acid–dimethylamine (SA–DMA) nucleation, fully including the effects of coagulation scavenging and cluster stability. Incorporating the new parameterization into 3-D chemical transport models, we achieved better consistencies between simulation results and observation data. This new parameterization provides new insights into atmospheric nucleation simulations and its effects on atmospheric pollution or health.
María Gonçalves Ageitos, Vincenzo Obiso, Ron L. Miller, Oriol Jorba, Martina Klose, Matt Dawson, Yves Balkanski, Jan Perlwitz, Sara Basart, Enza Di Tomaso, Jerónimo Escribano, Francesca Macchia, Gilbert Montané, Natalie M. Mahowald, Robert O. Green, David R. Thompson, and Carlos Pérez García-Pando
Atmos. Chem. Phys., 23, 8623–8657, https://doi.org/10.5194/acp-23-8623-2023, https://doi.org/10.5194/acp-23-8623-2023, 2023
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Dust aerosols affect our climate differently depending on their mineral composition. We include dust mineralogy in an atmospheric model considering two existing soil maps, which still have large associated uncertainties. The soil data and the distribution of the minerals in different aerosol sizes are key to our model performance. We find significant regional variations in climate-relevant variables, which supports including mineralogy in our current models and the need for improved soil maps.
Jianyan Lu, Sunling Gong, Jian Zhang, Jianmin Chen, Lei Zhang, and Chunhong Zhou
Atmos. Chem. Phys., 23, 8021–8037, https://doi.org/10.5194/acp-23-8021-2023, https://doi.org/10.5194/acp-23-8021-2023, 2023
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WRF/CUACE was used to assess the cloud chemistry contribution in China. Firstly, the CUACE cloud chemistry scheme was found to reproduce well the cloud processing and consumption of H2O2, O3, and SO2, as well as the increase of sulfate. Secondly, during cloud availability in December under a heavy pollution episode, sulfate production increased 60–95 % and SO2 was reduced by over 80 %. This study provides a way to analyze the phenomenon of overestimation of SO2 in many chemical transport models.
Laurent Menut, Arineh Cholakian, Guillaume Siour, Rémy Lapere, Romain Pennel, Sylvain Mailler, and Bertrand Bessagnet
Atmos. Chem. Phys., 23, 7281–7296, https://doi.org/10.5194/acp-23-7281-2023, https://doi.org/10.5194/acp-23-7281-2023, 2023
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This study is about the wildfires occurring in France during the summer 2022. We study the forest fires that took place in the Landes during the summer of 2022. We show the direct impact of these fires on the air quality, especially downstream of the smoke plume towards the Paris region. We quantify the impact of these fires on the pollutants peak concentrations and the possible exceedance of thresholds.
Hannah J. Rubin, Joshua S. Fu, Frank Dentener, Rui Li, Kan Huang, and Hongbo Fu
Atmos. Chem. Phys., 23, 7091–7102, https://doi.org/10.5194/acp-23-7091-2023, https://doi.org/10.5194/acp-23-7091-2023, 2023
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We update the 2010 global deposition budget for nitrogen (N) and sulfur (S) with new regional wet deposition measurements, improving the ensemble results of 11 global chemistry transport models from HTAP II. Our study demonstrates that a global measurement–model fusion approach can substantially improve N and S deposition model estimates at a regional scale and represents a step forward toward the WMO goal of global fusion products for accurately mapping harmful air pollution.
Chenxi Li, Yuyang Li, Xiaoxiao Li, Runlong Cai, Yaxin Fan, Xiaohui Qiao, Rujing Yin, Chao Yan, Yishuo Guo, Yongchun Liu, Jun Zheng, Veli-Matti Kerminen, Markku Kulmala, Huayun Xiao, and Jingkun Jiang
Atmos. Chem. Phys., 23, 6879–6896, https://doi.org/10.5194/acp-23-6879-2023, https://doi.org/10.5194/acp-23-6879-2023, 2023
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New particle formation and growth in polluted environments are not fully understood despite intensive research. We applied a cluster dynamics–multicomponent sectional model to simulate the new particle formation events observed in Beijing, China. The simulation approximately captures how the events evolve. Further diagnosis shows that the oxygenated organic molecules may have been under-detected, and modulating their abundance leads to significantly improved simulation–observation agreement.
Marianne Tronstad Lund, Gunnar Myhre, Ragnhild Bieltvedt Skeie, Bjørn Hallvard Samset, and Zbigniew Klimont
Atmos. Chem. Phys., 23, 6647–6662, https://doi.org/10.5194/acp-23-6647-2023, https://doi.org/10.5194/acp-23-6647-2023, 2023
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Here we show that differences, in magnitude and trend, between recent global anthropogenic emission inventories have a notable influence on simulated regional abundances of anthropogenic aerosol over the 1990–2019 period. This, in turn, affects estimates of radiative forcing. Our findings form a basis for comparing existing and upcoming studies on anthropogenic aerosols using different emission inventories.
Lei Kong, Xiao Tang, Jiang Zhu, Zifa Wang, Yele Sun, Pingqing Fu, Meng Gao, Huangjian Wu, Miaomiao Lu, Qian Wu, Shuyuan Huang, Wenxuan Sui, Jie Li, Xiaole Pan, Lin Wu, Hajime Akimoto, and Gregory R. Carmichael
Atmos. Chem. Phys., 23, 6217–6240, https://doi.org/10.5194/acp-23-6217-2023, https://doi.org/10.5194/acp-23-6217-2023, 2023
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A multi-air-pollutant inversion system has been developed in this study to estimate emission changes in China during COVID-19 lockdown. The results demonstrate that the lockdown is largely a nationwide road traffic control measure with NOx emissions decreasing by ~40 %. Emissions of other species only decreased by ~10 % due to smaller effects of lockdown on other sectors. Assessment results further indicate that the lockdown only had limited effects on the control of PM2.5 and O3 in China.
Ernesto Reyes-Villegas, Douglas Lowe, Jill S. Johnson, Kenneth S. Carslaw, Eoghan Darbyshire, Michael Flynn, James D. Allan, Hugh Coe, Ying Chen, Oliver Wild, Scott Archer-Nicholls, Alex Archibald, Siddhartha Singh, Manish Shrivastava, Rahul A. Zaveri, Vikas Singh, Gufran Beig, Ranjeet Sokhi, and Gordon McFiggans
Atmos. Chem. Phys., 23, 5763–5782, https://doi.org/10.5194/acp-23-5763-2023, https://doi.org/10.5194/acp-23-5763-2023, 2023
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Organic aerosols (OAs), their sources and their processes remain poorly understood. The volatility basis set (VBS) approach, implemented in air quality models such as WRF-Chem, can be a useful tool to describe primary OA (POA) production and aging. However, the main disadvantage is its complexity. We used a Gaussian process simulator to reproduce model results and to estimate the sources of model uncertainty. We do this by comparing the outputs with OA observations made at Delhi, India, in 2018.
Eleftherios Ioannidis, Kathy S. Law, Jean-Christophe Raut, Louis Marelle, Tatsuo Onishi, Rachel M. Kirpes, Lucia M. Upchurch, Thomas Tuch, Alfred Wiedensohler, Andreas Massling, Henrik Skov, Patricia K. Quinn, and Kerri A. Pratt
Atmos. Chem. Phys., 23, 5641–5678, https://doi.org/10.5194/acp-23-5641-2023, https://doi.org/10.5194/acp-23-5641-2023, 2023
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Remote and local anthropogenic emissions contribute to wintertime Arctic haze, with enhanced aerosol concentrations, but natural sources, which also contribute, are less well studied. Here, modelled wintertime sea-spray aerosols are improved in WRF-Chem over the wider Arctic by including updated wind speed and temperature-dependent treatments. As a result, anthropogenic nitrate aerosols are also improved. Open leads are confirmed to be the main source of sea-spray aerosols over northern Alaska.
Wenfu Tang, Simone Tilmes, David M. Lawrence, Fang Li, Cenlin He, Louisa K. Emmons, Rebecca R. Buchholz, and Lili Xia
Atmos. Chem. Phys., 23, 5467–5486, https://doi.org/10.5194/acp-23-5467-2023, https://doi.org/10.5194/acp-23-5467-2023, 2023
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Globally, total wildfire burned area is projected to increase over the 21st century under scenarios without geoengineering and decrease under the two geoengineering scenarios. Geoengineering reduces fire by decreasing surface temperature and wind speed and increasing relative humidity and soil water. However, geoengineering also yields reductions in precipitation, which offset some of the fire reduction.
Havala O. T. Pye, Bryan K. Place, Benjamin N. Murphy, Karl M. Seltzer, Emma L. D'Ambro, Christine Allen, Ivan R. Piletic, Sara Farrell, Rebecca H. Schwantes, Matthew M. Coggon, Emily Saunders, Lu Xu, Golam Sarwar, William T. Hutzell, Kristen M. Foley, George Pouliot, Jesse Bash, and William R. Stockwell
Atmos. Chem. Phys., 23, 5043–5099, https://doi.org/10.5194/acp-23-5043-2023, https://doi.org/10.5194/acp-23-5043-2023, 2023
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Chemical mechanisms describe how emissions from vehicles, vegetation, and other sources are chemically transformed in the atmosphere to secondary products including criteria and hazardous air pollutants. The Community Regional Atmospheric Chemistry Multiphase Mechanism integrates gas-phase radical chemistry with pathways to fine-particle mass. New species were implemented, resulting in a bottom-up representation of organic aerosol, which is required for accurate source attribution of pollutants.
Xuemei Wang, Hamish Gordon, Daniel P. Grosvenor, Meinrat O. Andreae, and Ken S. Carslaw
Atmos. Chem. Phys., 23, 4431–4461, https://doi.org/10.5194/acp-23-4431-2023, https://doi.org/10.5194/acp-23-4431-2023, 2023
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New particle formation in the upper troposphere is important for the global boundary layer aerosol population, and they can be transported downward in Amazonia. We use a global and a regional model to quantify the number of aerosols that are formed at high altitude and transported downward in a 1000 km region. We find that the majority of the aerosols are from outside the region. This suggests that the 1000 km region is unlikely to be a
closed loopfor aerosol formation, transport and growth.
Shixian Zhai, Daniel J. Jacob, Drew C. Pendergrass, Nadia K. Colombi, Viral Shah, Laura Hyesung Yang, Qiang Zhang, Shuxiao Wang, Hwajin Kim, Yele Sun, Jin-Soo Choi, Jin-Soo Park, Gan Luo, Fangqun Yu, Jung-Hun Woo, Younha Kim, Jack E. Dibb, Taehyoung Lee, Jin-Seok Han, Bruce E. Anderson, Ke Li, and Hong Liao
Atmos. Chem. Phys., 23, 4271–4281, https://doi.org/10.5194/acp-23-4271-2023, https://doi.org/10.5194/acp-23-4271-2023, 2023
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Anthropogenic fugitive dust in East Asia not only causes severe coarse particulate matter air pollution problems, but also affects fine particulate nitrate. Due to emission control efforts, coarse PM decreased steadily. We find that the decrease of coarse PM is a major driver for a lack of decrease of fine particulate nitrate, as it allows more nitric acid to form fine particulate nitrate. The continuing decrease of coarse PM requires more stringent ammonia and nitrogen oxides emission controls.
Jun-Wei Xu, Jintai Lin, Gan Luo, Jamiu Adeniran, and Hao Kong
Atmos. Chem. Phys., 23, 4149–4163, https://doi.org/10.5194/acp-23-4149-2023, https://doi.org/10.5194/acp-23-4149-2023, 2023
Short summary
Short summary
Research on the sources of Chinese PM2.5 pollution has focused on the contributions of China’s domestic emissions. However, the impact of foreign anthropogenic emissions has typically been simplified or neglected. Here we find that foreign anthropogenic emissions play an important role in Chinese PM2.5 pollution through chemical interactions between foreign-transported pollutants and China’s local emissions. Thus, foreign emission reductions are essential for improving Chinese air quality.
Kun Wang, Xiaoyan Ma, Rong Tian, and Fangqun Yu
Atmos. Chem. Phys., 23, 4091–4104, https://doi.org/10.5194/acp-23-4091-2023, https://doi.org/10.5194/acp-23-4091-2023, 2023
Short summary
Short summary
From 12 March to 6 April 2016 in Beijing, there were 11 typical new particle formation days, 13 non-event days, and 2 undefined days. We first analyzed the favorable background of new particle formation in Beijing and then conducted the simulations using four nucleation schemes based on a global chemistry transport model (GEOS-Chem) to understand the nucleation mechanism.
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Short summary
Large-scale enhancements of tropospheric BrO and the depletion of surface ozone are often observed in the springtime Arctic. Here, we use a chemical transport model to examine the role of sea salt aerosol from blowing snow in explaining these phenomena. We find that our simulation can account for the spatiotemporal variability of satellite observations of BrO. However, the model has difficulty in producing the magnitude of observed ozone depletion events.
Large-scale enhancements of tropospheric BrO and the depletion of surface ozone are often...
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